• Korean Journal of Mineralogy and Petrology
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• v.36 no.4
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• pp.313-321
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• 2023

Numerous studies have investigated the adsorptive sequestration of radioactive cesium in the natural environment. Among these studies, adsorption onto minerals and high-temperature treatment stand out as highly effective, as demonstrated by the use of zeolite. In this study, cesium was ion-exchanged with birnessite and subsequently underwent high-temperature treatment up to 1100℃ to investigate both mineral phase transformation and the leaching characteristics of cesium. Birnessite has a layered structure consisting of MnO₆ octahedrons that share edges, demonstrating excellent cation adsorption capacity. The high-temperature treatment of cesium-ion-exchanged birnessite resulted in changes in the mineral phase, progressing from cryptomelane, bixbyite, birnessite to hausmannite as the temperature increased. This differs from the phase transformation observed in the tunneled manganese oxide mineral todorokite ion-exchanged with cesium, which shows phase transformation only to birnessite and hausmannite. The leaching of cesium from cesium-ion-exchanged birnessite was estimated by varying the reaction time using both distilled water and a 1 M NaCl solution. The leaching quantity changed according to the treatment temperature, reaction time, and type of reaction solution. Specifically, the cesium leaching was higher in the sample reacted with 1 M NaCl compared to the sample with distilled water and also increased with longer reaction time. For the samples reacted with distilled water, the cesium leaching initially increased and then decreased, while in the NaCl solution, the leaching decreased, increased again, and finally nearly stopped like the sample in the distilled water for the sample treated at 1100℃. These changes in leaching are closely associated with the mineral phases formed at different temperatures. The phase transformation to cryptomelane and birnessite enhanced cesium leaching, whereas bixbyite and hausmannite hindered leaching. Notably, hausmannite, the most stable phase occurring at the highest temperature, demonstrated the greatest ability to inhibit cesium leaching. This results strongly suggest that high-temperature treatment of cesium-ion-exchanged birnessite effectively immobilizes and sequesters cesium.

• Proceedings of the Korean Radioactive Waste Society Conference
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• 2003.11a
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• pp.21-31
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• 2003

IAEA, FT-04-020, and ANS 16.1, standard leaching test methods, were evaluated comparatively with their test results. Leaching index of Co-60 and Cs-137 for all waste forms were above 6.0. Their leaching behavior were contrary according to the type of matrix and leachant. Leachability of Co in cement waste form was higher in simulated seawater than demi. water, and higher in demi. water in paraffin waste form. Leachability of Cs was contrary to Cs. Cumulative fraction leached of Co was higher such as IAEA＞ANS＞FT in cement waste form.

• Journal of Radiation Protection and Research
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• v.11 no.2
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• pp.91-103
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• 1986

Experimental study for the leaching behavior of Cs-137 was carried out using the simulated evaporator bottom product of PWR plant. The method of leach test proposed by the IAEA was partially modified using ANS method. The effect of various factors, i.e., sampling method, curing temperature, curing time, leachant temperature, vermiculite addition and volume-to-surface ratio, was considered in this experiment. Diffusion model in semi-infinite slab was in a good agreement with the data obtained from 4-weeks cured specimens. The effective diffusion coefficient of the specimens which were cured at the temperature of $24^{\circ}C$ for 4 weeks was found to be $1.20{\sim}1.47{\times}10^{-11}cm^2/sec$. With the experimentally obtained diffusion coefficient ($1.47{\times}10^{-11}cm^2/sec$), long-term prediction for the leaching of Cs-137 was carried out using finite-slab approximation. The estimated fraction of Cs-137 which remains in the environment is found to be less than 0.25 percent of initial amount after 100 years. About 25 years after the beginning of leaching, its fractional amount in the environment reachs the maximum value, 0.66 percent of initial amount.

• Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT)
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• v.1 no.1
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• pp.93-103
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• 2003

IAEA, FT-04-020, and ANS 16.1, standard leaching test methods, were evaluated comparatively with their test results. Leaching index of $^{60}$ Co and $^{137}$ Cs by ANS 16.1 method for waste forms of paraffin and cement were above 6.0. Their leaching behavior were depending on the type of matrix and leachant. Leachability of $^{60}$ Co for cement waste form was higher in simulated seawater than do-mineralized water, and was higher in de-mineralized water for paraffin waste form. leachability of $^{60}$ Co was contrary to $^{137}$ Cs. Cumulative fraction leached of $^{60}$ Co was higher in order or IAEA ＞ ANS ＞ FT in a cement waste form.

• Journal of Radiation Protection and Research
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• v.10 no.2
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• pp.113-121
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• 1985

For the safety assessment of radwaste treatment and disposal, the leaching characteristics of $Cs^+\;and\;Sr^{++}$ from the cement-solidified radwastes was investigated by means of the survey and analysis of the activity leach rate and cumulative leach fraction of $^{137}Cs\;and\;^{90}Sr$ leaching from solidified radwastes. The cylindrical cement-solidified samples were made by the sodium silicate method and neutralization method changing the mole density of simulated liquid radwaste, type of cement, adding material and concentration of boric acid. The leaching study was carried out by the method using simulated PWR concentrated liquid radwaste solidified in cement that had been processed following the recommendations of IAEA. All the experimental results are in well accordance with the research data reported previously, but the watertight cement-solidified radwastes show rather high leach rate of radioactivity. It is learned, therefore, that the watertight cement is not adequate as the material for the solidified radwastes.

• Nuclear Engineering and Technology
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• v.55 no.10
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• pp.3617-3627
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• 2023

This study presents a method to solidify spent ion-exchange resin (IER) in a metakaolin-based geopolymer and shows results of mechanical strength, immersion, leaching, irradiation, and thermal cycling tests for waste acceptance criteria (WAC) to repository. The geopolymer waste form with 20 wt% of simulated spent IER met the WAC in South Korea (ROK), and the leaching tests of various sized-waste forms up to 15.0 × 30.0 cm and waste loadings up to 20 wt% for 1-5 d and 1-90 d achieved a leachability index, L_i > 6. In a leaching test for 5 d, the cumulative fraction leached (CFL) for Cs, which leached the most, was linearly correlated with the square root of leaching time for all waste forms, and L_i increased as the size of the waste form increased. The CFL was also correlated with elapsed time in the 90 d leaching test. The correlations among CFL, time, and volume-to-surface area ratio of waste forms used to estimate the L_i of Cs of a 200-L sized geopolymer with 15 wt% IER showed the L_i values as 14.73 (5 d) and 17.71 (90 d), respectively, indicating that the large-sized geopolymer waste form met the WAC.

• Nuclear Engineering and Technology
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• v.23 no.4
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• pp.374-386
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• 1991

Various factors affecting the teachability of Cs-137 in cement matrix have been investigated. Factors investigated include such as pressure curing, vibration curing, pressure leaching, the effect of the clay addition, ion-exchange resin(IRN-77) addition, and $CO_2$or air injection. Leaching experiments were conducted by the method recommended by IAEA. To analyze the experimental results, pore structure analysis of cement matrices was carried out by BET method. Cement matrices may not contact directly with underground water in real repository, since the surroundings of disposed drums are filled with backfill. Thus, the effect of backfill to the teachability has been investigated. The well-known diffusion theory was utilized to predict long term leach rate and cumulative fraction leached of Cs-137 or non-radioactive species.

• Korean Journal of Environmental Agriculture
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• v.15 no.2
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• pp.198-206
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• 1996

Leaching of $^{54}Mn$, $^{60}Co$, $^{85}Sr$ and $^{137}Cs$ in paddy soil was studied using lysimeter cultures in a greenhouse. The radionuclides were applied to the water surfaces shortly before transplanting and five different times between transplanting and harvest. Fertilizer KCl and slaked lime were added simultaneously in the rate of 83kg and 200kg, respectively, per l0a following the first application after transplanting. Percolating water was sampled until two days before harvest. Concentrations of the radionuclides in percolating water decreased in the order of $^{85}Sr$ > $^{54}Mn$ > $^{60}Co$ > $^{137}Cs$ on the whole. Time taken to reach the maximum was the shortest for $^{137}Cs$(< one week) and the longest for $^{54}Mn$ and $^{85}Sr$. Six days' water dropping started 47 days after transplanting reduced the concentrations of $^{54}Mn$, $^{60}Co$, $^{85}Sr$ and $^{137}Cs$ by factors of 30-180, 3-75, 2-4 and 3-6, respectively, depending on the application time. After the significant decrease, $^{54}Mn$ concentration tended to gradually increase but $^{137}Cs$ did to the contrary Percent leaching varied 0.09-6.2% for $^{54}Mn$, 0.009-0.9% for $^{60}Co$, 1.4-14.4% for $^{85}Sr$ and 0.002-0.06% for $^{137}Cs$, with the application time. The highest leaching came from the application at 40 days after transplanting for all the radionuclides. The addition of KCl and lime increased percent leaching of the radionuclides by factors of 9, 85, 4 and 9, respectively.

• Nuclear Engineering and Technology
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• v.22 no.4
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• pp.315-325
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• 1990

The analytical repository source term (REPS) computer code is developed for the safety assessment of radioactive waste geologic repository. For reliable prediction of the leach rates for various radionuclides, degradation of concrete structures, corrosion rate of waste container, degree of corrosion on the container surface, and the characteristics of radionuclides are considered in this REPS code. For the validation of the radionuclide leach rates predicted by the REPS model, the calculated leach rates of Cs-137, Sr-85, and Co-60 are compared with two reported leaching test results. Cesium and strontium leach congruently, and the leaching test results of these species can be reproduced by the congruent leaching model included in the REPS model. In case of cobalt, the solid diffusion model is in good agreement with the leaching test results.

• Korean Journal of Mineralogy and Petrology
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• v.36 no.1
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• pp.33-40
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• 2023

Todorokite is a manganese oxide mineral containing Mg²⁺ in a tunnel structure in which MnO₆ octahedra share corners. In order to investigate the suitability and efficiency of high temperature-treated todorokite as a material for adsorption and fixation of Cs, Cs was ion exchanged and the amount of leached Cs from todorokite was measured. The todorokite used in this study was synthesized by transforming Na-birnessite to Mg-buserite and used as a precursor. After high temperature treatment, Cs exchanged todorokite changed to birnessite and hausmannite as the temperature increased. The amount of leached Cs was investigated for Cs exchanged todorokite which was reacted with distilled water and 1 M NaCl solution at different reaction times. In general, for the samples reacted with 1 M NaCl solution, the fixation of Cs was quite effective, although the amount of leached Cs was greater due to the ion exchange reaction with Na. As the treatment temperature increased, the amount of leached Cs increased and then decreased again, which was related to the mineral phases formed at each temperature. As birnessite was formed, the amount of leached Cs increased, but as birnessite decreased, that decreased again. As the mineral phase changed to hausemanite, the amount of Cs decreased rapidly. The results of our study show that Cs exchanged todorokite can be used as a material that effectively fixes Cs and prevents its diffusion by high temperature treatment.