The nuclear fuel that melted during the Fukushima nuclear accident in 2011 is still being cooled by water. In this process, contaminated water containing radioactive substances such as cesium and strontium is generated. The total amount of radioactive pollutants released by the natural environment due to the nuclear accident in Fukushima in 2011 is estimated to be 900 PBq, of which 10 to 37 PBq for cesium. Radioactive cesium (137Cs) is a potassium analog that exists in the water in the form of cations with similar daytime behavior and a small hydration radius and is recognized as a radioactive nuclide that has the greatest impact on the environment due to its long half-life (about 30 years), high solubility and diffusion coefficient, and gamma-ray emission. In this study, alginate beads were designed using Prussian blue, known as a material that selectively adsorbs cesium for removal and detection of cesium. To confirm the adsorption performance of the produced Prussian blue, immersion experiments were conducted using Cs standard solution, and MCNP simulations were performed by modeling 1L reservoir to conduct experiments using radioactive Cs in the future. An adsorption experiment was conducted with water containing standard cesium solution using alginate beads impregnated with Prussian blue. The adsorption experiment tested how much cesium of the same concentration was adsorbed over time. As a result, it was found that Prussian blue beads removed about 80% of cesium within 10-15 minutes. In addition, MCNP simulation was performed using a 1 L reservoir and a 3inch NaI detector to optimize the amount of Prussian blue. The results of comparing the efficiency according to the Prussian volume was shown. It showed that our designed system holds great promise for the cleanup and detection of radioactive cesium contaminated seawater around nuclear plants and/or after nuclear accidents. Thus, this work is expected to provide insights into the fundamental MCNP simulation based optimization of Prussian blue for cesium removal and this work based MCNP simulation will pave the way for various practical applications.

After the Fukushima accident in 2011, relevant concerns regarding the contamination of the natural environment rose abruptly. For example, water contaminated by radionuclides such as Cs and Sr may directly flow into the ocean and threaten the marine ecosystem. In this respect, costeffective and efficient decontamination techniques need to be developed and verified to remediate the contaminated water. Prussian blue (PB) is known as a representative material that can adsorb Cs by ion-trapping and is widely used for medical purposes. However, there is a limitation that PB itself is non-separable and highly mobile in aqueous system, so it needs a fixture, such as bentonite, to be collected after the adsorption. Furthermore, while the performance of PB toward Cs is relatively well known, its behavior toward Sr has rarely been reported. The object of this study is to investigate the sorption characteristics of Cs and Sr onto PB-functionalized bentonite at various conditions. The adsorbent employed in the present work was prepared by mixing bentonite, FeCl3, and K4[Fe(CN)6] at room temperature for 24 hours in the aqueous solution. The concentrations of FeCl3 and K4[Fe(CN)6] were set to a range of 5-200 % compared to the cation exchange capacity of bentonite. After that, the PB-functionalized bentonite was sieved with a mesh size of 63 μm and then reacted with the Cs and Sr solution at various liquid-to-solid (L/S) ratios of 2-10 g/L for up to 500 minutes. Moreover, synthetic seawater containing additional Cs and Sr was reacted with PBfunctionalized bentonite to characterize the ion selectivity of PB. After the completion of the adsorption experiment, a part of the adsorbent was separated and desorption of Cs and Sr with 2 M of nitric acid was performed. For the quantification of aqueous Cs and Sr concentrations, ICP-MS was employed after the filtration with a pore size of 0.45 μm. The result obtained in this study revealed a high sorption affinity of Cs and Sr onto PBfunctionalized bentonite. The analysis results also presented that the sorption reactions of Cs and Sr reached their steady state within 10 minutes of reaction time. Furthermore, the ion selectivity toward Cs and Sr was verified through sorption test with synthetic seawater. According to the high sorption affinity and selectivity, the PB-functionalized bentonite synthesized through this study is expected to be widely used for remediating the Cs- and Sr-contaminated groundwater and seawater, particularly in nuclear waste-relevant industries.

Prussian blue is known as a superior material for selective adsorption of radioactive cesium ions; however, the separation of Prussian blue from aqueous suspension, due to particle size of around several tens of nanometers, is a hurdle that must be overcome. Therefore, this study aims to develop granule type adsorbent material containing Prussian blue in order to selectively adsorb and remove radioactive cesium in water. The surface of granular activated carbon was grafted using a covalent organic polymer (COP-19) in order to enhance Prussian blue immobilization. To maximize the degree of immobilization and minimize subsequent detachment of Prussian blue, several immobilization pathways were evaluated. As a result, the highest cesium adsorption performance was achieved when Prussian blue was synthesized in-situ without solid-liquid separation step during synthesis. The sample obtained under optimal conditions was further analyzed by scanning electron microscope-energy dispersive spectrometry, and it was confirmed that Prussian blue, which is about 9.7% of the total weight, was fixed on the surface of the activated carbon; this level of fixing represented a two-fold improvement compared to before COP-19 modification. In addition, an elution test was carried out to evaluate the stability of Prussian blue. Leaching of Prussian blue and cesium decreased by 1/2 and 1/3, respectively, compared to those levels before modification, showing increased stability due to COP-19 grafting. The Prussian blue based adsorbent material developed in this study is expected to be useful as a decontamination material to mitigate the release of radioactive materials.

프러시안 블루 유사체(Prussian Blue Analogue : PBA)는 3차원 구조와 기공을 갖는 금속-유 기골격체이며, 유기 리간드의 종류에 따라 다양한 구조를 갖는다. PBA는 바이오센서, 광학, 촉매, 수소 저장 장치 등의 분야에서 주목 받고 있으며 화학적 안정성을 가진 환경 친화적인 물질이다. 또한 다양 한 크기의 미세기공을 조정할 수 있어 흡착분야에서 많이 활용되고 있다. 본 연구는 수열합성법을 이용 하여 금속유기골격체인 Mn3[Fe(CN)6]2를 합성하였다. 전구체로 K4[Fe(CN)6]와 MnCl2를 사용하였고, 합 성된 물질은 소성하여 망간철산화물을 생성하였다. 실험 변수로 전구용액의 pH, 전구체의 몰농도, 반응 시간을 조절하여 입자의 크기와 형태에 대한 영향을 확인하였다. 합성된 다공체는 XRD, SEM, FT-IR, UV-Vis, TG/DTA에 의해 분석하였고, 여러 염료에 대한 흡착 특성을 평가하였다.