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Youngho Sihn,Chan Woo Park,In-Ho Yoon,Hee-Man Yang,Ilgook Kim 한국방사성폐기물학회 2022 한국방사성폐기물학회 학술논문요약집 Vol.20 No.1
Detritiation of low-level tritiated water has become global issue after Fukushima accident. Several attempts have been made to reduce the radioactivity of Fukushima tritiated water below legal limit of nuclear plant effluents (~104 Bq·L?1). Various technologies such as water distillation, electrolysis, and catalytic exchange were tested to treat the tritiated water, however, those demand enormous expense to achieve the goal due to low process efficiency. It highlights that the performance enhancement of current technologies is necessary to improve economic feasibility. We have quantitatively evaluated the separation performance of various polymers toward low-level tritium (~105 Bq·L?1) through batch experiments. The polystyrene with grafted by 20 types of functional groups (Tris (2-aminoethyl) amine, dimethylaminomethyl, isocyanate, mercaptomethyl, aminomethyl, hydroxymethyl, triphenylphosphine, morpholine, 2-chlorotrityl amine, 4-(dimethylamino) pyridine, poly (vinyl chloride) carboxylated, poly (4-vinyl pyridine), p-toluenesulfonic acid, p-toluenesulfonyl hydrazide, piperidine, acetyl polystyrene, 2-chlorotrityl chloride, piperazine, diethylene triamine, poly (vinyl chloride)) were suspended in HTO solution (initial activity = 4.7 × 105 Bq·L?1). After the equilibration, the suspension was filtered using 3 kDa membrane filter and the activity in filtrates were quantified by LSC (HIDEX-300 SL). The results demonstrate the detritiation efficiency and separation factors of functional groups toward tritium. Carboxylic group (COOH) showed the most reactive performance as detritiation efficiency of ~4%. Compared to other functional groups, styrene sulfonyl groups including sulfonyl amide (SNH2) and sulfonyl hydrazide (SNHNH2) revealed promising performance for tritium separation as separation factor of 10.97 and 3.85, respectively. However, sulfonyl hydroxide (SOH) which is known as reactive functional group to tritium exchange showed the poor performance (detritiation efficiency: 0.68%; separation factor: 3.02). This study could suggest the promising functional groups for detritiation of low-level tritiated water which can be utilized to enhance the performance of current technologies. For example, reactive functional groups can be grafted on the surface of packing material within distillation tower resulting in the increasing detritiation efficiency.
Molecular Identification of Cr(VI) Removal Mechanism on Vivianite Surface
Bae, Sungjun,Sihn, Youngho,Kyung, Daeseung,Yoon, Sunho,Eom, Taedaehyeong,Kaplan, Ugras,Kim, Hyungjun,Schä,fer, Thorsten,Han, Seunghee,Lee, Woojin American Chemical Society 2018 Environmental science & technology Vol.52 No.18
<P>Experimental and theoretical studies were conducted to identify the molecular-scale reaction mechanism for Cr(VI) removal by a ferrous phosphate mineral, vivianite. The surface-normalized rate constant for Cr(VI) removal in a vivianite suspension at pH 7 was higher than those obtained for other Fe(II)-containing minerals (i.e., magnetite and pyrite). The highest rate constant was obtained at pH 5, which was 35- and 264-times higher than those obtained at pH 7 and 9, respectively, indicating the dramatic acceleration of removal kinetics with decreasing pH of suspension. The X-ray photoelectron spectroscopy (XPS) and X-ray absorption near-edge structure (XANES) spectroscopy revealed that Cr(VI) removal involved reduction of Cr(VI) to Cr(III) coupled with oxidation of Fe(II) to Fe(III) on the vivianite surface. In addition, the density functional theory (DFT)-optimized structure of the Cr(VI)-vivianite complex was consistent with that obtained from extended X-ray absorption fine structure (EXAFS) spectroscopy and revealed the transformation of vivianite to amorphous Fe(III) phosphate. We also demonstrated that both Cr(VI) species, HCrO<SUB>4</SUB>̅ and CrO<SUB>4</SUB><SUP>2-</SUP>, can effectively bind to the vivianite surface, particularly on the Fe sites having 6 neighboring Fe molecules with 4 H<SUB>2</SUB>O and 2 PO<SUB>4</SUB> moieties. Our results show that Cr(VI) is readily reduced to Cr(III) by vivianite via adsorption and inner-sphere complexation, suggesting that in anoxic iron-phosphate-enriched environments, vivianite may significantly influence the fate and transport of Cr(VI).</P> [FIG OMISSION]</BR>
Hydrogen isotope exchange behavior of protonated lithium metal compounds
Park, Chan Woo,Kim, Sung-Wook,Sihn, Youngho,Yang, Hee-Man,Kim, Ilgook,Lee, Kwang Se,Roh, Changhyun,Yoon, In-Ho Korean Nuclear Society 2021 Nuclear Engineering and Technology Vol.53 No.8
The exchange behaviors of hydrogen isotopes between protonated lithium metal compounds and deuterated water or tritiated water were investigated. The various protonated lithium metal compounds were prepared by acid treatment of lithium metal compounds with different crystal structures and metal compositions. The protonated lithium metal compounds could more effectively reduce the deuterium concentration in water compared with the corresponding pristine lithium metal compounds. The H<sup>+</sup> in the protonated lithium metal compounds was speculated to be more readily exchangeable with hydrons in the aqueous solution compared with Li<sup>+</sup> in the pristine lithium metal compounds, and the exchanged heavier isotopes were speculated to be more stably retained in the crystal structure compared with the light protons. When the tritiated water (157.7 kBq/kg) was reacted with the protonated lithium metal compounds, the protonated lithium manganese nickel cobalt oxide was found to adsorb and retain twice as much tritium (163.9 Bq/g) as the protonated lithium manganese oxide (69.9 Bq/g) and the protonated lithium cobalt oxide (75.1 Bq/g) in the equilibrium state.
In-Ho Yoon,Ilgook Kim,KwanSeong Jeong,Youngho Sihn,Chan Woo Park,Geun-Ho Kim 한국방사성폐기물학회 2023 한국방사성폐기물학회 학술논문요약집 Vol.21 No.2
The operation of nuclear facilities involves the potential for on-site contamination of soil, primarily resulting from pipe leaks and other operational incidents. Globally, decommissioning process for commercial nuclear power plants have revealed huge-amounts of soil waste contaminated with Cs-137, Sr-90, Co-60, and H-3. For example, Connecticut Yankee in the United States produced approximately 52,800 ton of contaminated soil waste, constituting 10% of the total waste generated during its decommissioning. Environmental remediation costs associated with nuclear decommissioning in the US averaged $60 million per unit, representing a significant 10% of the whole decommissioning expenses. Consequently, this study undertook a preliminary investigation to identify important factors for establishing a site remediation strategy based on radionuclide- and site-specific media- characteristics, focusing the efficiency enhancement for the environmental remediation. The factors considered for this investigation were categorized into physical/environmental, socioeconomic, technical, and management aspects. Physical/environmental factors contained the site characteristics, contamination levels, and environmental sensitivity, while socio-economic factors included the social concerns and economic costs. Technical and management factors included subcategories such as technical considerations, policy aspects, and management factors. Especially, technical factors were further subdivided to consider the site reuse potential, secondary waste generation by site remediation, remediation efficiency, and remediation time. Additionally, our study focused the key factors that facilitate the systematic planning for the site remediation, considering the distribution coefficient (Kd) and hydrogeological characteristics associated with each radionuclide in specific site conditions. Therefore, key factors in this study focus the geochemical characteristics of site media including the particle size distribution, chemical composition, organic and inorganic constituents, and soil moisture content. Moreover, the adsorption properties of site media were examined concerning the distribution coefficient (Kd) of radionuclides and their migration characteristics. Furthermore, this study supported the development of a conceptual framework, containing the remediation strategies that incorporate the mobility of radionuclides, according to the site-specific media. This conceptual framework would necessitate the spatial analysis techniques involving the whole contamination surveys and radionuclide mobility modeling data. By integrating these key factors, the study provides the selection and simulation of optimal remediation methods, ultimately offering the estimated amounts of radioactive waste and its disposal costs. Therefore, these key factors offer foundational insights for designing the site remediation strategies according the sitespecific information such as the distribution coefficient (Kd) and hydrogeological characteristics.
Exploring the Potential of Zeolites for Selective Separation of Hydrogen Isotopes
In-Ho Yoon,Chan Woo Park,Hyung-Ju Kim,Ilgook Kim,Youngho Sihn,Hee-Man Yang 한국방사성폐기물학회 2023 한국방사성폐기물학회 학술논문요약집 Vol.21 No.1
The physicochemical similarities of hydrogen isotopes have made their separation a challenging task. Conventional methods such as cryogenic distillation, Girdler sulfide process, chromatography, and thermal cycling absorption have low separation factors and are energy-intensive. To overcome these limitations, research has focused on kinetic quantum sieving (KQS) and chemical affinity quantum sieving (CAQS) effects for selective separation of hydrogen isotopes. Porous materials such as metal-organic frameworks (MOF), covalent organic frameworks (COF), zeolites, carbon, and organic cages have been studied for hydrogen separation. This study have the literature review for previous research on D2/H2 adsorption and analyzes the D2/H2 adsorption behaviors of hydrogen isotopes for various zeolite using BET at 77 K. The study predicts the D2/H2 adsorption selectivity based on the results obtained with BET. These hydrogen isotope adsorption fundamentals provide a foundation for future processes for tritium separation.