The mobility and transport of radioactive cesium are crucial factors to consider for the safety assessment of high-level radioactive waste disposal sites in granite. The retardation of radionuclides in the fractured crystalline rock is mainly controlled by the hydrochemical condition of groundwater and surface reactions with minerals present in the fractures. This paper reports the experimental results of cesium sorption to the Wonju Granite, a typical Mesozoic granite in Korea, performed in an anaerobic chamber that mimics the anoxic environment of a deep disposal site. We measured the rates and amounts of cesium (133Cs) removed by crushed granite samples in different electrolyte (NaCl, KCl, and CaCl2) solutions and a synthetic groundwater solution, with variations in the initial cesium concentration (10-5, 5×10-6, 10-6, 5×10-7 M). The cesium sorption kinetic and isotherm data were successfully simulated by the pseudo-second-order kinetic model (r2= 0.99) and the Freundlich isotherm model (r2= 0.99), respectively. The sorption distribution coefficient of granite increased almost linearly with increasing biotite content in granite samples, indicating that biotite is an effective cesium scavenger. The cesium removal was minimal in KCl solution compared to that in NaCl or CaCl2 solution, regardless of the ionic strength and initial cesium concentration that we examined, showing that K+ is the most competitive ion against cesium in sorption to granite. Because it is the main source mineral of K+ in fracture fluids, biotite may also hinder the sorption of cesium, which warrants further research.
The final disposal of spent nuclear fuel(SNF) from nuclear power plants takes place in a deep geological repository. The metal canister encasing the SNF is made of cast iron and copper, and is engineered to effectively isolate radioactive isotopes for a long period of time. The SNF is further shielded by a multi-barrier disposal system comprising both engineering and natural barriers. The deep disposal environment gradually changes to an anaerobic reducing environment. In this environment, sulfide is one of the most probable substances to induce corrosion of copper canister. Stress-corrosion cracking(SCC) triggered by sulfide can carry substantial implications for the integrity of the copper canister, potentially posing a significant threat to the long-term safety of the deep disposal repository. Sulfate can exist in various forms within the deep disposal environment or be introduced from the geosphere. Sulfate has the potential to be transformed into sulfide by sulfate-reducing bacteria(SRB), and this converted sulfide can contribute to the corrosion of the copper canister. Bentonite, which is considered as a potential material for buffering and backfilling, contains oxidized sulfate minerals such as gypsum(CaSO4). If there is sufficient space for microorganisms to thrive in the deep disposal environment and if electron donors such as organic carbon are adequately supplied, sulfate can be converted to sulfide through microbial activity. However, the majority of the sulfides generated in the deep disposal system or introduced from the geosphere will be intercepted by the buffer, with only a small amount reaching the metal canister. Pyrite, one of the potential sulfide minerals present in the deep disposal environment, can generate sulfates during the dissolution process, thereby contributing to the corrosion of the copper canister. However, the quantity of oxidation byproducts from pyrite is anticipated to be minimal due to its extremely low solubility. Moreover, the migration of these oxidized byproducts to the metal canister will be restricted by the low hydraulic conductivity of saturated bentonite. We have comprehensively analyzed and summarized key research cases related to the presence of sulfates, reduction processes, and the formation and behavior characteristics of sulfides and pyrite in the deep disposal environment. Our objective was to gain an understanding of the impact of sulfates and sulfides on the long-term safety of high-level radioactive waste disposal repository.
Jaehoon Choi;SunJu Park;Hyunsoo Seo;Hyun Tai Ahn;Jeong-Hwan Lee;Junghoon Park;Seong-Taek Yun
Economic and Environmental Geology
/
v.56
no.6
/
pp.847-870
/
2023
The safe disposal of high-level radioactive waste requires accurate predictions of the long-term geochemical behavior of radionuclides. To achieve this, the present study was conducted to model geochemical behaviors of uranium (U), plutonium (Pu), and palladium (Pd) under different hydrogeochemical conditions that represent deep groundwater in Korea. Geochemical modeling was performed for five types of South Korean deep groundwater environment: high-TDS saline groundwater (G1), low-pH CO2-rich groundwater (G2), high-pH alkaline groundwater (G3), sulfate-rich groundwater (G4), and dilute (fresh) groundwater (G5). Under the pH and Eh (redox potential) ranges of 3 to 12 and ±0.2 V, respectively, the solubility and speciation of U, Pu, and Pd in deep groundwater were predicted. The result reveals that U(IV) exhibits high solubility within the neutral to alkaline pH range, even in reducing environment with Eh down to -0.2 V. Such high solubility of U is primarily attributed to the formation of Ca-U-CO3 complexes, which is important in both G2 located along fault zones and G3 occurring in granitic bedrocks. On the other hand, the solubility of Pu is found to be highly dependent on pH, with the lowest solubility in neutral to alkaline conditions. The predominant species are Pu(IV) and Pu(III) and their removal is predicted to occur by sorption. Considering the migration by colloids, however, the role of colloid formation and migration are expected to promote the Pu mobility, especially in deep groundwater of G3 and G5 which have low ionic strengths. Palladium (Pd) exhibits the low solubility due to the precipitation as sulfides in reducing conditions. In oxidizing condition, anionic complexes such as Pd(OH)3-, PdCl3(OH)2-, PdCl42-, and Pd(CO3)22- would be removed by sorption onto metal (hydro)oxides. This study will improve the understanding of the fate and transport of radionuclides in deep groundwater conditions of South Korea and therefore contributes to develop strategies for safe high-level radioactive waste disposal.
Kim, Ho-Yong;Choi, In-Gyu;Ahn, Sye-Hee;Oh, Sei-Chang;Hong, Chang-Young;Min, Byeong-Cheol;Yang, In
Journal of the Korean Wood Science and Technology
/
v.36
no.1
/
pp.110-123
/
2008
The use of CCA as a wood preservative was recently inhibited due to its environmental pollution and human harmfulness. Instead of CCA, copper azole (CuAz) and alkaline copper quaternary (ACQ) have been used as alternative wood preservatives, but the price of the preservatives is much more expensive than that of CCA. As a substitute for high-priced CuAz and ACQ, environmentally friendly wood preservatives were formulated with okara, which is an organic waste from the production of tofu. Prior to formulating the preservatives, okara was hydrolyzed by three levels of sulfuric acid concentration (1, 2.5 and 5%) to easily penetrate the effective components of the preservatives into wood blocks. Final preservative solutions were formulated with the hydrolyzed okara and metal salts, such as copper sulfate, copper chloride and borax. The preservatives were treated into wood blocks by vacuum-pressure method to measure the treatability of the preservatives, and the treated wood blocks were placed in hot water for three days to measure the leachability of the preservatives. The effective components of the preservatives might be successfully penetrated into wood blocks through the uses of hydrolyzed okara and ammonia water. However, the leached amount of effective components was increased as the concentration of acid used for the hydrolysis of okara increased. The treatability and leachability of the preservatives were not affected by hydrolysis temperature but negatively affected by the addition of borax. Based on the results above, the optimal conditions for formulating okara-based wood preservatives cost-effectively and environmentally might be 1% acid hydrolysis of okara and the use of $CuCl_2$ as a metal salt. In addition, the treatability and leachability of okara-based wood preservatives were superior or no differences comparing with those of CuAz. Therefore, it is concluded that okara-based wood preservatives might have a potential to be used as an environmentally friendly wood preservative.
Batch scale experiments to investigate the efficiency of the solidification process for metal mine tailing treatment were performed. Portland and MSG (micro silica pouting) cements were used as solidifier and three kinds of mine tailings (located at Gishi, Daeryang, and Aujeon mine) were mixed with cements to paste solidified matrices. Single axis com-pressible strengths of solidified matrices were measured and their heavy metal extraction ratios were calculated to investigate the solidification efficiency of solidified matrices created in experiments. Solidified matrices ($5cm{\times}5cm{\times}5cm$) were molded from the paste of tailing and cements at various conditions such as different tailing/cement ratio, cement/water ratio, and different cement or tailing types. Compressible strengths of solidified matrices after 7, 14, and 28 day cementation were measured and their strengths ranged from 1 to $2kgf/mm^2$, which were higher than Korean limit of compressible strength for the inside wall of the isolated landfill facility ($0.21kgf/mm^2$). Heavy metal extractions from intact tailings and powdered matrices by using the weak acidic solution were performed. As concentration of extraction solution for the powdered solidified matrix (Portland cement + Gishi tailing at 1:1 w.t. ratio) decreased down to 9.7 mg/L, which was one fifth of As extraction concentration for intact Gishi tailings. Pb extraction concentration of the solidified matrix also decreased to lower than one fourth of intact tailing extraction concentration. Heavy metal extraction batch experiments by using various pH conditions of solution were also performed to investigate the solidification efficiency reducing heavy metal extraction rate from the solidified matrix. With pH 1 and 13 of solution, Zn and Pb concentration of solution were over the groundwater tolerance limit, but at pH $1{\sim}13$ of solution, heavy metal concentrations dramatically decreased and were lower than the groundwater tolerance limit. While the solidified matrix was immerged Into very acidic or basic solution (pH 1 and 13), pH of solution changed to $9{\sim}10$ because of the buffering effect of the matrix. It was suggested that the continuous extraction of heavy metals from the solidified matrix is limited even in the extremely high or low pH of contact water. Results of experiments suggested that the solidification process by using Portland and MSG cements has a great possibility to treat heavy metal contaminated mine tailing.
Laboratory leaching experiment study carried out to estimate a extent of heavy metals that could be leached out when acid rain(pH 5.0-3.0) and strong acidic solution(pH 2.5-1.0) reacted with tailings and contaminated soils from abandoned metal mines. In slightly to moderately acid conditions(pH 5.0-3.0), As, Pb and Zn dissolutions became significantly increased with decreased pH in tailing, while dissolution of these elements was very limited in contaminated soil. These results suggested that moderately acid rainwater leaches Pb, As and Zn from the tailings, while these elements would remain fixed in contaminated soil. In the pH range of 2.5-1.0(strongly acid condition), Zn, Cd and Cu concentrations of leachate rapidly increased with decreased pH in contaminated soil, while Pb, As and Co dissolutions became importantly increased in tailings. The experimental solubility of Zn. Cd and Cu was very low even at very low pH values(up to pH 1), except for CY4(Cheongyang mine). These can result from an incomplete dissolution or the presence of less soluble mineral phases. So, the solubility of heavy metals depends not only on the pH values of leachate but also on the speciation of metals associated with contaminated soils and tailings. The relative mobility of each element within failings at the pH 5.0-3.0 of the reaction solution was in the order of Pb>Zn>Cd>Co=Cu>As. In case of pH 2.5-1.0 of the reaction solution, the relative mobility of each element within contaminated soils and tailings were in the order of Zn>Cd>Cu>Co>Pb=As for contaminated soils, and Pb>Zn>Cd>hs>Co>Cu for tailings. The obtained results could be useful for assessing the environmental effects and setting up the restoration plan in the areas.
The effects of $Al_2$O$_3$ addition upon the sintering range of clay-EAF dust (the specified wastes produced from steel making process) system body which would be used as a constructing bricks were investigated. The slope of apparent density to sintering temperature decreased for Clay-dust body containing 5~15 wt% A1203 sintered at 1200-125$0^{\circ}C$, and the absorption(%) of specimen sintered above 125$0^{\circ}C$ decreased due to the formation of open pores produced by pore bloating. For the specimen without any $Al_2$O$_3$ addition sintered at 1275$^{\circ}C$, the major phase was cristobalite, the small amount of mullite (3Al$_2$O$_3$ 2SiO$_2$) formed and the hematite (Fe$_2$O$_3$) remained. In the Clay-dust system body containing $Al_2$O$_3$ 15 wt%, however, the cristobalite disappeared and the major phase was mullite. Also the part of $Al_2$O$_3$ reacted with hematite to form hercynite (FeAl$_2$O$_4$). From the these results, addition of $Al_2$O$_3$ to Clay-dust system body enlarges a sintering range; decreasing an apparent density and absorption slop to sintering temperature owing to consumption of liquid phase SiO$_2$ at higher temperature and gas-forming component Fe$_2$O$_3$ at reduced atmosphere which would decrease an amount of liquid formed and increase the viscosity of the liquid produced during the sintering process.
This study was carried out to prepare information for the establishment of countermeasures for an area contaminated with minewaste from an old zinc mine at Kahak-long in Kwangmyong. Minewaste and bottom sediments from the streams in this area were sampled and were analyzed for Cd, Cu, Pb, and Zn extracted with different solution. Total heavy metal contents in both minewaste and bottom sediments were fairly high. Cadmium and Zn contents in the minewaste and Cd, Cu, Pb, and Zn contents in the bottom sediments extracted with 0.1 N HCl showed a much higher level than those in the background level of paddy soils and in the soils around the other metal mines regardless of the distance from the mine. Sulfide/residue forms of Cd, Cu, Pb, and Zn covered the highest portions for the minewaste. For bottom sediments, sulfide/residue forms of Cu and Zn formed the highest portions, whereas the contents of both carbonate and sulfide/residue forms of Cd and Pb were significant. The lower the pH of the extracting solutions, the more heavy metals extracted from both minewaste and bottom sediments.
The element arsenic, which is abundant in the Earth's crust, is used for various industrial purposes including materials for disease treatment and household goods. Various human activities, such as the disposal of soil waste, metal mining and smelting, and combustion of fossil fuels, have caused the pollution of the environment with arsenic. Recently, guidelines for arsenic in rice have been adopted by the Korean ministry of food and drug safety to prevent health risks based on rice consumption. Because of the exposure to arsenic and its accumulation in the human body through various channels, such as air inhalation, skin contact, ingestion of drinking water, and food consumption, integrated multimedia risk assessment is required to adopt appropriate risk management policies. Therefore, integrated human health risk assessment was carried out in this study using integrated exposure assessment based on multimedia (e.g., air, water, and soil) and multi-route (e.g., oral, inhalation, and dermal) scenarios. The results show that oral uptake via drinking water is the most common pathway of arsenic into the human body, accounting for 57%-96% of the total arsenic exposure. Among various age groups, the highest exposures to arsenic were observed in infants because the body weight of infants is low and the surface areas of infant bodies are large. Based on the results of the exposure assessment, the cancer and non-cancer risks were calculated. The cancer risk for CTE and RME is in the range of 2.3E-05 to 6.7E-05 and thus is negligible because it does not exceed the cancer probability of 1.0E-04 for all age groups. On the other hand, the cancer risk for RME varies from 6.4E-05 to 1.8E-04 and from 1.3E-04 to 1.8E-04 for infants and preschool children, exceeding the excess cancer risk of 1.0E-04. The non-cancer risks range from 5.4E-02 to 1.9E-01 and from 1.5E-01 to 6.8E-01, respectively. They do not exceed the hazard index 1 for all scenarios and all ages.
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