최근 전기차 시장의 확장으로 배터리 산업이 급격히 성장함에 따라 폐배터리 리사이클링 기술 개발의 필요성이 증가하고 있다. 폐배터리 리사이클링 기술은 배터리 산업에 핵심적인 리튬, 코발트, 니켈 등 희소금속의 공급을 안정화하고 환경 및 인간의 건강에 미치는 영향을 경감할 수 있다. 본 총설에서는 금속 회수 기술의 배경이 되는 이론적 원리와 현재 상 용되고 있는 금속 회수 공정을 소개하고자 한다. 또한, 기존 공정의 문제점을 개선하려는 연구 및 기술 개발 동향을 서술하여 리사이클링 기술이 나아가야 할 방향을 소개하고자 한다.

Various radioactive metal wastes are generated during operation and decommissioning of nuclear facilities. Radioactive metal wastes with complex geometries or volumetric contamination can be difficult to decontaminate and disposal costs may increase. To solve these problems, the radioactive metal wastes can be treated by melting method. In this study, we designed a melting furnace system of air induction melting type, which is widely utilized due to its advantages of good thermal efficiency, uniform heating and guaranteed safety for radioactive material. By utilizing the melting furnace system, volatile radionuclides existed in the base material can be captured in the form of gas or dust by the filter. The radionuclides whose chemical properties can easily form metal oxides present as slag. For this reason, the specific radioactivity of the base material can be reduced. Radionuclides that are difficult to transport to slag and dust are uniformly distributed in the base material. A dedicated power supply and a transformer were necessary to be included in the melting furnace system since the induction furnace uses high-frequency currents. In addition, a hood is placed on top of the furnace to capture fumes generated during melting, and additional hoods were installed around the furnace to remove airborne dust. In particular, a dust collection unit consisting of a cyclone and a HEPA filter were constructed to effectively collect dust containing radionuclides. During the melting process, the slag is removed and accumulated separately, and the ingot production system was designed to produce the ingot using molten metal. The furnace was constructed for tilting the molten metal by moving the furnace using hydraulic system. The water cooling system and cooling tower were prepared to cool off the equipment with high temperature during melting is cooled off. The above process was specified in the operating procedure developed for this melting furnace system, and the operator shall operate and inspect according to the prescribed procedures. The radioactivity concentration in the sample taken in the step of tilting shall be analyzed whether they meet clearance level for self-disposal determined and publicly announced by the Commission. We can conduct self-disposal for the product of melting furnace system confirmed by the Commission as having the radioactivity concentration by nuclide not exceeding the value determined by the Commission.

Decommissioning of a nuclear power plant (NPP) generate large amounts of various types of wastes. In accordance with the Nuclear Safety and Security Commission Notice of Korea (No. 2020- 6), they are classified as High Level Waste (HLW), Intermediate Level Waste (ILW), Low Level Waste (LLW), Very Low Level Waste (VLLW) and Exempt Waste (EW) according to specific activities. More than 90% of the wastes are at exempt level, mostly metal and concrete wastes with low radioactivity, of which the concentrations of nuclides is less than the allowable concentration of self-disposal. The self-disposal or recycling of these wastes is widely used worldwide. More than 10,000 drums, based on 200 L drum, are expected to be produced in the decommissioning process of a unit of nuclear power plant. Due to the limited storage capacity of the intermediate & low level waste disposal facility in Gyeongju, recycling and self-disposal of EW are actively recommended in Korea. A variety of scenarios were proposed for recycling and self-disposal of decommissioning metal/ concrete wastes, and a computational program called REDISA was developed to perform the dose evaluation for each recycling and self-disposal scenario. The REDISA computer program can calculate external and internal exposure doses by simulating the exposure pathways from waste generation, thru transport, processing, manufacture, to the final destination of recycling or self-disposal. In this study, the self-disposal scenario was only considered for the dose evaluation. Many studies have been conducted to evaluate the exposure doses of the radioactive waste disposal sites. However, there have been few researches on dose evaluation for self-disposal landfills. In particular, the dose evaluation is important not only during the operation period, but also for a long period after the facility is closed. To this end, we developed a conceptual model for dose evaluation for post-closure scenarios of the self-disposal landfill of decommissioning metal/concrete wastes with reference to the methodology of IAEA-TECDOC-1380. The model incorporates three exposure pathways, including external exposure from contaminated soil, internal exposure by inhalation, and internal exposure by ingestion of water and food grown in contaminated soil. The duration of the dose evaluation is set to 100,000 years after the closure of landfill facility. Co-60 was selected as dominant nuclide, and dose evaluation was performed based on unit specific activity of 1 Bq/g. Exposure doses shall be verified for their application in accordance with the annual dose limit of 10 Sv/yr for self-disposal. As a result, the post-closure scenario of selfdisposal landfills have shown negligible effects on public health, which means that the exposures doses from transportation and operational processes should be considered more carefully for selfdisposal of decommissioning metal/concrete wastes.

Organic waste generated by small and medium-sized (S&M-sized) metal decontamination in NPP decommissioning. To lower the concentration of these organic substances for a level acceptable at the disposal site, the project of “Development of Treatment Process of Organic Decontamination Liquid Wastes from Decommissioning of Nuclear Power Plants” is being carried out. The conditioning and treatment process of organic liquid waste was designed. Also, the literature was investigated to make simulated organic liquid waste, and the composition of these waste was analyzed and compared. As the decontamination agent, organic acids such as EDTA, oxalic acid, citric acid are used. The sum of the concentrations of these organic materials was set to a maximum value of 1,000 ppm. The major metal ions of the decontamination liquid waste estimated are 59Fe, 51Cr, 54Mn, 63Ni, and the concentrations are respectively 527, 163, 161, 159 ppm. Additional major metal ions are 60Co, 58Co, 137Cs. 58Co is replaced by 60Co because it has the same chemical properties as 60Co. Unlike the HLW, the contamination level of S&M-sized metal in primary system was quite low, so 60Co is set to 2,000 Bq/g. Considering the contribution of fission and gamma ray dose constant, 137Cs was estimated to 360 Bq/g. Also, suspended solids of decontamination liquid waste were set at 500 ppm. Under these assumptions, the simulated organic liquid waste was made, and then organic substances and metal ions were analyzed with TOC analyzer and ICP-OES. The TOC analysis value was expected to 392 ppm in consideration of the equivalent organic quantity. the test result was 302 ppm. Some of organics appears to have been decomposed by acid. The values of metal ions (Fe3+, Cr3+, Mn2+, Ni2+) analyzed by ICP-OES are 139, 4, 152, 158 ppm, respectively. A large amount of Cr3+ and Fe3+ were expected to exist as ions, but they existed in the form of suspended solid. Mn2+ and Ni2+ came out similar to the expected values. The designed conditioning and treatment process is largely divided into pretreatment, conditioning, and decomposition processes. After collecting in the primary liquid waste storage tank, large particulate impurities and suspensions are removed through a pretreatment process. In the conditioning process, treated liquid waste passes through UF/RO membrane system, and pure water is discharged to the environment after monitoring. Concentrated water is decomposed in the electrochemical catalyst decomposition process, then this water secondarily passes through the RO membrane system and then discharged to the environment after monitoring. Through an additional experiment, the conditioning and treatment process will be verified.

In this study, the current situation of recycling domestic and foreign metal clearance waste was reviewed to suggest the optimal recycling scenario for metal clearance waste that occurs the most when decommission nuclear power plants. Factors that can directly or indirectly affect the recycling of metal clearance waste were analyzed and evaluation criteria that can be used to evaluate optimal recycling measures were prepared. Using this, a scenario for recycling the optimal metal clearance waste suitable for the domestic environment was proposed. As a result of comparing/reviewing the importance of the first level of the evaluation criteria, public acceptance, national policy, and regulatory requirements were evaluated as the most important ones, and recycling acceptance and regulatory requirements were evaluated as the most important the second level of evaluation criteria. As a result of reviewing the clearance waste recycling scenario, it was evaluated that unrestricted recycling scenario was preferred. This may be because the survey subjects are composed of experts in the nuclear power field, so they know recycling of clearance waste in general industries does not significantly affect radiation safety. However even if it is clearance waste, the public may feel reluctant to recycle just because it was discharged from nuclear power plants, so policy and institutional improvements are needed to reassure the public along with the scientific safety of clearance waste. In addition, in order to improve public acceptance, it seems necessary to prepare specific measures to ensure the participation of public in the entire decommissioning process, share related information, and disclose all routes from generation to disposal of decommissioning waste. Considering that research on domestic clearance waste recycling options has not been activated, this study is significant in that it derives a scenario for recycling metal clearance waste that can be implemented. Also, it is expected that the evaluation criteria derived from this study will be used significantly when establishing a radioactive waste management strategy.

High-intensity focused ultrasonic (HIFU) decontamination technology to decontaminate complex metal radioactive waste was developed and verified. Ultrasonic decontamination technology is a method widely used in this field, but its energy strength is weak, so it cannot be applied to fixed contamination. The HIFU developed in this study can eliminate a wide range of fixed contamination due to the advantage of maintaining a high frequency while having hundreds of times the energy intensity compared to conventional general ultrasonic method. In addition, there is a merit in that there is no work that generates a lot of secondary wastes such as chemical decontamination method or threatens the safety of workers. In particular, high ultrasonic energy is transmitted to curved parts and inside pipes that cannot be decontaminated with blasting method, so various types of metal wastes can be treated with the HIFU method. In this study, the performance of the HIFU was verified for zirconium chips, and the radioactivity after decontamination was reduced to less than MDA in all subjects.

The treatment of piggery wastes was carried out at pilot scale using a multilayered metal-activated carbon system followed by carbon bed filtration. The physicochemical properties were obtained from treated samples with aqueous solutions containing metallic ions such as Ag+, Cu2+, Na+, K+ and Mn2+, which main obsevations are subjected to inspect surface properties, color removal properties by Uv/Vis and EDX. Multilayered metal-activated carbons were contacted with waste water to investigation of the simultaneous catalytic effect for the COD, BOD, T-N and T-P removal. The removal results for the piggery waste using multilayered metal-activated carbon bed was achieved the satisfactory removal performance under permitted values of Ministry of Environment of Korea. The high efficiency of the multilayered metal-activated carbon bed was determined by the performance of this material for trapping, catalytic effect and adsorption of organic solid particles.

원자력시설의 해체 시 발생되는 금속폐기물의 양은 전 세계적으로 향후 50년 동안 스테인레스강 약 95 만톤, 탄소강 870 만 톤, 구리 220 만 톤으로 총 1,200 만 톤 정도 발생할 것으로 예측되고 있다. 해체 시 발생하는 금속 조각은 대부분 방사능에 아주 미미하게 오염되어 있기 때문에 이중에서 대부분은 무구속 방출이나 약간의 제염 처리 후 일정한 공정을 거쳐 핵 시설내의 폐기물 저장 용기나 처분 상자, 폐기물 드럼, ISO 컨테이너 등으로 재활용되고 있거나, 앞으로 재활용할 수 있다고 보고되고 있다. 국내 원자력시설 해체 시 다량으로 발생될 것으로 예상되는 금속 조각을 수용하기에는 폐기물 처리장이 매우 부족할 뿐만 아니라, 지속적으로 처분 단가의 증가가 예상되므로 이러한 문제를 해결하기 위해서 방사성 금속폐기물의 효과적인 감용 및 재활용 기술이 요구되고 있다. 금속 폐기물의 감용 및 재활용 기술 중 현재까지 가장 적절한 기술로서 용융 기술이 있다. 유럽을 주축으로 미국과 일본에서 활발히 연구되어져 온 용융 기술은 다른 처분 방법에 비해 부피 감용비가 가장 높아 최종처분시설 공간을 절약할 수 있으며 탄소강, 스테인레스강 및 인코넬 등 많은 양의 금속을 회수하는 것이 가능하다. 또한, 이 기술은 휘발성 핵종(Cs 등)이나 금속과 반응성이 적은 핵종(U, Pu 등)을 슬래그 속에 포집하여 제염하거나, 방사성 핵종들이 주괴에 균일하게 분포하고 금속의 결정 격자속에 고정화시킬 수 있기 때문에 보다 안정화시킬 수 있다는 장점들을 가지고 있다.

The purpose of this study was to suggest feasible disposal methods for heavy-metal-contaminated soil or mine tailings through solidification/stabilization. To improve the compressive strength and enhance the heavy-metal stabilization after solidification/stabilization, we used the industrial wastes (oyster shell powder and waste gypsum) and indigenous bacteria as immobilization agents. Three indigenous bacteria were isolated from each heavy-metal-contaminated soil or mine tailing site, and the bacteria were identified by cellular fatty acid composition analysis. The results of cellular fatty acid composition analysis showed that the closest strains of these bacteria are Brevibacillus centrosporus, Lysinibacillus sphaericus, and Bacillus megaterium. To the best of our knowledge, this research was the first report of biomineralization by Brevibacillus centrosporus. As a result of mixing additives with the optimum mixing ratio suggested in this study, the compressive strengths of specimens were satisfied in accordance with the US Environmental Protection Agency (EPA) waste treatment standard after 28 days of aging. Additionally, the results of the Toxicity Characteristics Leaching Procedure (TCLP) and Synthetic Precipitation Leaching Procedure (SPLP) analysis showed the successful immobilization of heavy metals after 28 days of specimen formation for solidification/stabilization.