The initial radionuclide migration quantity depends on the total amount of solubilized species. Geochemical modeling based on a thermodynamic database (TDB) has been employed to assess the solubility of radionuclides. It is necessary to evaluate whether the TDB describes the domestic repository conditions appropriately. An effective way to validate the TDB-based modeling results is through direct comparisons with experimentally measured values under the conditions of interest. Here, the solubilities of trivalent Sm, Eu, and Am were measured in synthetic KURT-DB3 groundwater (Syn- DB3) and compared with modeling results based on ThermoChimie TDB. Ln2(CO3)3·xH2O(cr) (Ln = Sm, Eu) solids were introduced into the Syn-DB3 and dissolved Sm and Eu concentrations were monitored over 223 days. X-ray diffraction analysis confirmed that the crystallinity of the solid compounds was maintained throughout the experiments. The dissolved Sm and Eu concentrations at equilibrium were close to the predicted solubilities of Sm2(CO3)3(s) and Eu2(CO3)3(s) based on the ThermoChimie TDB. The Am solubility measured under oversaturated conditions was comparable to the measured Eu concentrations, although they were measured under different experimental settings. More experimental data are needed for Am-carbonate solid systems with careful characterization of the solid phases to better evaluate Am solubility in domestic groundwater conditions.
The growing significance of sustainable energy technologies underscores the need for safe and efficient management of spent nuclear fuels (SNFs), particularly via deep geological disposal (DGD). DGD involves the long-term isolation of SNFs from the biosphere to ensure public safety and environmental protection, necessitating materials with high corrosion resistance for DGD canisters. This study investigated the feasibility of a Cu–Ni film, fabricated via additive manufacturing (AM), as a corrosion-resistant layer for DGD canister applications. A wire-fed AM technique was used to deposit a millimeter-scale Cu–Ni film onto a carbon steel (CS) substrate. Electrochemical analyses were conducted using aerated groundwater from the KAERI underground research tunnel (KURT) as an electrolyte with an NaCl additive to characterize the oxic corrosion behavior of the Cu–Ni film. The results demonstrated that the AM-fabricated Cu–Ni film exhibited enhanced corrosion resistance (manifested as lower corrosion current density and formation of a dense passive layer) in an NaCl-supplemented groundwater solution. Extensive investigations are necessary to elucidate microstructural performance, mechanical properties, and corrosion resistance in the presence of various corroding agents to simplify the implementation of this technology for DGD canisters.
기후변화에 따라 수자원의 취약성이 증가하고 있고, 그로 인해 지하수 자원의 필요성이 강조되고 있다. 특히, 낙동강권역이 자리 잡은 한반도 남부는 매년 봄 가뭄과 같은 물 부족 현상이 빈번하게 발생하고 있다. 물 부족의 대안 으로 지하수 자원 이용이 대두되고 있으나, 지하수 자원의 활용에는 수질 안정성이 반드시 요구된다. 이 연구는 2023년 8월과 10월, 2회에 걸쳐 낙동강 하류 광려천 유역을 대상으로 지하수 관정 총 54개소와 하천수 총 5개의 지점에서 시 료를 채취하여 현장 수질 및 실내 수질 분석을 수행하였다. 현장에서 측정한 전기전도도의 값은 지하수와 하천수 모두 연구 지역 수계 하류로 갈수록 농도가 증가하는 경향을 보여 준다. 이는 하류의 농업 활동이 하천수에 직접적으로 유 입됨을 지시한다. 실내 수질 분석 결과 연구 지역의 수질 유형은 주로 [Ca-HCO3] 유형이 가장 많고, [Ca-SO4] 유형이 그 뒤를 이었다. 8월과 10월 시간에 따른 수질 유형의 변화를 확인하면, Ca 함량이 우세한 지역이 Na 함량이 우세한 지역으로 변화하고, 이러한 지하수 관정은 주로 하류에 위치하고 있음을 확인하였다. 결국 연구 지역 하류의 하천수·지 하수의 농도 변화는 공장단지, 폐수 처리시설, 농경지의 분포 현황 및 낙동강 하류의 유입과 밀접한 관계가 있고, 이를 통해 인위적인 오염이 발생하였음을 유추할 수 있다.
To secure approval for a decommissioning plan in Korea, it is essential to evaluate contamination dispersion through groundwater during the decommissioning process. To achieve this, licensees must assess the groundwater characteristics of the facility’s site and subsequently develop a groundwater flow model. It is worth noting that Combustible Radioactive Waste Treatment Facility (CRWTF) is characterized by their simplicity and absence of liquid radioactive waste generation. Given these facility characteristics, the groundwater flow model for CRWTF utilizes data from neighboring facilities, with the feasibility of using reference data substantiated through comparative analysis involving groundwater characteristic testing and on-site modeling. To enable a comparison between the actual site’s groundwater characteristics and the referenced modeling, two types of hydraulic constant characterization tests were conducted. First, hydraulic conductivity was determined through long-term pumping and recovery tests. The ‘Theis’ and ‘Cooper-Jacob’ equations, along with the ‘Theis recovery’ equation, were applied to calculate hydraulic conductivity, and the final result adopted the average of the calculated values. Secondly, a groundwater flow test was conducted to confirm the alignment between the main flow direction of the referenced model and the groundwater flow in the CRWTF, utilizing the particle tracking technique. The evaluation of hydraulic conductivity from the hydraulic constant test revealed that the measured value at the actual site was approximately 1.84 times higher than the modeled value. This variance is considered valid, taking into consideration the modeling’s calibration range and the fact that measurements were taken during a period characterized by wet conditions. Furthermore, a close correspondence was observed between the groundwater flow direction in the reference model (ranging from 90° to 170°) and the facility’s actual flow direction (ranging from 78° to 95°). The results of reference data for the CRWTF, based on the nearby facility’s model, were validated through the hydraulic properties test. Consequently, the modeling data can be employed for the demolition plan of CRWTF. It is also anticipated that these comparative analysis methods will be instrumental in shaping the groundwater investigation plans for facilities with characteristics similar to CRWTF.
This study presents distribution of naturally occurring radioactive materials in groundwater in Jeju island. Radon (222Rn) and potassium (40K) concentrations were performed by using Liquid Scintillation Counter and Ion Chromatograph respectively. In addition, the activities of uranium and thorium nuclides were analyzed by Inductively Coupled Plasma Mass Spectroscopy. Groundwater samples were collected from 9 sites of water intake facilities for wide area supply in Jeju island from September 2022 to September 2023. The 40K concentrations of groundwater ranged between 0.050 and 0.400 Bq·L-1. The radon concentrations in groundwater were in the range of 0 to 60 Bq L-1, and there was no groundwater exceeding the range of 148 Bq L-1 proposed by the US EPA. The distribution of uranium and thorium in groundwater varied from 0 to 500 ng L-1 and 0 to 2.4 ng L-1, respectively. The concentrations of uranium did not exceed 30 μg L-1, thresholds indicated by the US EPA. By analyzing the concentrations of 40K, 222Rn, 238U and 232Th, the annual effective dose of residents can be assessed. The evaluated residents’ effective dose from natural radionuclides due to intake of drinking water is less than the recommended value of 100 μSv y-1. Consequently, this study indicates that the cancer risks of the residents in Jeju island from naturally occurring radioactive materials ingested with water is insignificant.
The mobility of radionuclides in the subsurface environment is governed by a interaction of radioactivity characteristics and geochemical conditions with adsorption reactions playing a critical role. This study investigates the characteristics and mechanisms of radionuclides adsorption on site media in viewpoint of nuclear safety, particularly focusing on the potential effect of seawater infiltration in coastal site near nuclear power plant. Seawater intrusion alters the chemistry in groundwater, including parameters such as pH, redox potential, and ionic strength, thereby affecting the behavior of radionuclides. To assess the safety of site near nuclear power plant and the environmental implications of nuclide leakage, this research conducted various experiments to evaluate the behavior of radionuclides in the subsurface environment. High distribution coefficients (50-2,500 ml/g) were observed at 10 mg/L Co, with montmorillonite > hydrobiotite > illite > kaolinite. It decreased with competing cations (Ca2+) and was found to decrease significantly by 90% with a decrease in pH to 4. It is believed that the adsorption capacity of cationic radionuclides decreases significantly as the clay mineral surface becomes less negatively charged. For Cs, the distribution coefficient (180-560 ml/g) was higher for montmorillonite > hydrobiotite > illite > kaolinite. Compared to Co, it was found to be less influenced by pH and more influenced by competing cations. For Sr, the distribution coefficient (100-380 ml/g) was higher in the order of hydrobiotite > montmorillonite > illite > kaolinite. Compared to Cs, it was found to be less affected by pH and also less affected by the effect of competing cations compared to Cs. Seawater samples from Gampo and Uljin site near Nuclear Power Plant in Korea were analyzed to determine their chemical composition, which was subsequently used in adsorption experiments. Additionally, the seawater-infiltrated groundwater was synthesized in laboratory according to previous literature. The study focused on the adsorption and behavior of three key radionuclides such as cesium, strontium, and cobalt onto four low permeability media (clay minerals) such as kaolinite, illite, hydrobiotite, and montmorillonite known for their high adsorption capacity at a site of nuclear power plant. At concentrations of 5 and 10 mg/L, the adsorption coefficients followed the order of cobalt > cesium > strontium for each radionuclide. Notably, the distribution coefficient (Kd) values exhibited higher values in seawater-infiltrated groundwater environments compared to seawater with relatively high ionic strength. Cobalt exhibited a substantial adsorption coefficient, with a marked decrease in Kd values in seawater conditions due to elevated ionic strength. In contrast, cesium displayed less dependency on seawater compared to other radionuclides, suggesting distinct adsorption mechanisms, possibly involving fractured edge sites (FES) in clay. Strontium exhibited a significant reduction in adsorption in seawater compared to groundwater in all Kd sorption experiments. The adsorption data of cobalt, cesium, and strontium on clay minerals in contact with seawater and seawater-infiltrated solutions offer valuable insights for assessing radioactive contamination of groundwater beneath coastal site near nuclear power plant sites. This research provides a foundation for enhancing the safety assessment protocols of nuclear power plant sites, considering the potential effects of seawater infiltration on radionuclide behavior in the subsurface environment.
The disposal of spent nuclear fuel (SNF) in a deep geological repository (DGR) is a widely accepted strategy for the long-term sequestration of radiotoxic SNF. Ensuring the safety of a DGR requires the prediction of various reactions and migration behaviors of radionuclides (RNs) present in SNF within its geochemical surroundings. Understanding the dissolution behaviors of mineral phases harboring these RNs is crucial, as the levels of RNs in groundwater are basically linked to the solubility of these solid phases. Accurate measurements of solubility demand the use of welldefined solid materials characterized by chemical compositions and structures. Herein, we attempted the synthesis of sklodowskite, a magnesium-uranyl (U(VI))-silicate, employing a twostep hydrothermal synthetic approach documented previously. Subsequently, we subjected this synthesized sklodowskite to various analytical techniques, including powder X-ray diffraction (pXRD), scanning electron microscopy/energy dispersive X-ray spectrometry (SEM/EDX), and vibrational spectroscopies (FTIR and Raman). Based on our findings, we confidently identify the obtained mineral phase as sklodowskite (Mg[UO2SiO3OH]2·5H2O). This identification is primarily based on the similarity between its pXRD pattern and the reference XRD pattern of sklodowskite. Furthermore, the measured infrared and Raman spectra show the vibrational modes of UO2 2+ and SiO4 4- ions, particularly within the 700~1,100 cm-1 region, which support that the synthetic mineral has a characteristic layered uranyl-silicate structure of crystalline sklodowskite. Finally, we utilized synthetic minerals to estimate its solubility up to about three months in a model groundwater, where the dissolved species composition is analogous to that of granitic groundwater from the KAERI Underground Research Tunnel. In this presentation, we will present in detail the results of spectroscopic characterizations and the methodology employed to assess the solubility of the U(VI)-silicate solid phase.
Currently, Korea is considering a disposal system based on Sweden’s KBS-3 model to dispose of high-level waste. The disposal system uses a multi-barrier concept to protect high-level waste with canister, buffer, backfill, and natural rock. In Korea, copper and iron are being considered for external and internal canisters, and bentonite is being considered as a buffer material. This is a similar choice to many overseas disposal systems. However, unlike the rolling, extrusion, and forging manufacturing methods being considered overseas for manufacturing external canister, domestic research is currently underway on manufacturing external copper canister using cold spray coating. The canister manufacturing method may vary depending on unit cost and manufacturing convenience. However, the properties of metal vary slightly depending on the manufacturing method of the metal. In this case, the characteristics of the canister may vary slightly depending on the canister manufacturing method, and eventually the corrosion resistance may also vary slightly. In order to understand how the copper canister manufacturing method affects corrosion resistance, corrosion rates were calculated and compared through electrochemical corrosion experiments at domestic groundwater ion concentration.
The mobility of uranium (U) in various disposal environments of a deep geological repository is controlled by various geochemical conditions and parameters. In particular, oxidation state of uranium is considered as a major factor to control the mobility of uranium in most of geological environments. In this study, therefore, we investigated the geochemical behaviors of uranium in grounwater samples from natural analogue study sites located in the Ogcheon Metamorphic Belt (OMB). Groundwater samples were taken using a packer system from Boeun Hoenam-myun site and Geumsan Suyoung-ri site where several boreholes were dilled with various depths. The geochemical properties and parameters such as temperature, pH, Eh, EC, and DO were directly measured in the site using an in-line measurement method. The concentrations of major cations and anions in the groundwater samples were measured by using ICP-OES (Inductively Coupled Plasma-Optical Emission Spectrometry) and IC (Ion Chromatography), respectively. The concentrations of trace elements including U and Th were measured by using ICP-MS (Inductively Coupled Plasma-Mass Spectrometry) The concentrations of U in the groundwater samples are very low for the Hoenammyun site (0.03~0.69 ppb) and Suyoung-ro site (0.39~1.74 ppb) even though the two sites are uranium deposits and redox conditions are weakly oxidizing. The speciation, saturation index (SI), pH-Eh (Poubaix) diagram were calculated using the Geochemist’s Workbench (GWB 9.0) program and the recent OECD/NEA thermochemical database for U. Calculation results for U speciation in the groundwater samples show that major dissolved uranium species in the groundwater samples are mainly as calcium uranyl carbonate complexes such as Ca2UO2(CO3)3(aq) and CaUO2(CO3)3 2- for almost all groundwater samples. The calculated results for SI and Poubaix diagram also show that the dominant uranium solid phase is a uranyl silicate mineral, uranophane (Ca(H2O)(UVIO2)2 (SiO2)2(OH)6), not uraninite (UIVO2). Since the determination of Eh values for natural groundwater samples is very difficult and uncertain work, we analyzed and discussed the effect of Eh on the geochemical behaviors of U in the groundwater. However, these calculation results are not consistent with the observation for U minerals in rock samples using electron microscopic techniques. Thus, we need further studies to explain the discrepancy between calculation and observation results.
This study investigates the behavior of bentonite, used as a buffer material in deep geological disposal systems, in the context of pore morphology under the influence of field-collected groundwater conditions. The bentonite was processed into block form using cold isostatic press (CIP) and subsequently analyzed for its pore morphology in situ using synchrotron X-ray computed tomography (CT) within the field-collected groundwater environment. Bentonite buffers play a critical role in deep geological disposal systems by preventing contact between disposal containers and groundwater. Bentonite typically exhibits swelling upon contact with water, forming few layers of water molecules between its structural layers. However, the presence of ions such as K+ and Cl- can lead to a sharp reduction in swelling pressure. Loss of swelling pressure could negatively impact the integrity of future deep geological disposal systems, making its assessment crucial. This study involves processing various types of bentonite, including natural Na-type bentonite, into block forms and subjecting them to exposure in both deionized water and field-collected groundwater conditions. Internal pore morphology changes were measured using Xray CT technology.
This study explores strategies to address the variability of heat energy using renewable energy and heat grids to achieve carbon neutrality. Renewable energy source introduce fluctuations that can impact the stability of power systems, while heat grids provide a systematic infrastructure for efficient supply of heat energy and power generation. Jeju Island is chosen as a case study, focusing on balance control based on groundwater-based geothermal energy to optimize the distribution of heat energy. The results demonstrate that the 3rd control method is the most effective in maintaining the target temperature in greenhouses, and specific temperature settings and objectives are proposed for each control method based on crop requirements. These research findings contribute to achieving carbon neutrality and reducing power consumption.
Shallow groundwater in rural areas is primarily polluted by agricultural activities. Nitrate-nitrogen is an indicator of artificial pollution. In this study, the hydrochemical characteristics and nitrate-nitrogen pollution of shallow groundwater were examined in two agricultural villages (Hyogyo-ri and Sinan-ri) in Chungcheongnam-do Province, Korea. Physicochemical quality analysis of shallow groundwater and stream water in the field, and chemical analysis in the laboratory were conducted from July 2020 to October 2021. In Hygyo-ri and Sinan-ri villages, shallow groundwater mainly b elonged t o the C a-Cl, Ca-H CO3, Na-HCO3, and Na-Cl types, whereas stream water predominantly belonged to the Ca-HCO3 type. The nitrate-nitrogen concentration in shallow groundwater varied depending on the season, displaying an increased concentration of nitrate-nitrogen in the dry season compared to the rainy season. Stream water may be influenced by runoff into villages from the surrounding area, although both shallow groundwater and stream water are affected by artificial pollution. In addition, the nitrate-nitrogen concentration in stream water was lower than that in shallow groundwater.
Solubility and species distributions of radionuclides in domestic groundwater conditions are required for the safety assessment of deep underground disposal system of spent nuclear fuel (SNF). Minor actinides including Am contribute significant extents to the long-term radiotoxicity of SNF. In this study, the solubility of Am was evaluated in synthetic groundwater (Syn-DB3), which were simulated for the groundwater of the DB3 site in the KAERI Underground Research Tunnel (KURT). Geochemical modeling was performed based on the ThermoChimie_11a (2022) thermochemical database from Andra to estimate the solubility and species distributions of Am in the Syn-DB3 condition. Dissolved Am concentrations in the Syn-DB3 were experimentally measured under oversaturation conditions. Am(III) stock solution in perchlorate media was sequentially diluted in Syn-DB3 to prepare 8 μM Am(III) in Syn-DB3. The pH of the solutions was adjusted to be in the range of 6.4–10.5. A portion of the samples was transferred to quartz cells for UV-Vis absorption and time-resolved laser fluorescence spectroscopy studies and the rest were stored in centrifuge tubes. The absorption spectra of the samples were monitored over 70 days and the results suggest that Am colloidal particles were formed initially in all the samples and precipitated rapidly within two days. Over the experimental period of 236 days, small volume (10 μL) of the samples in the centrifuge tubes were periodically withdrawn after centrifugation (18000 rpm, 1 hr) for the liquid scintillation counting to measure the concentrations of Am dissolved in Syn-DB3. In the end of the experiments, pH of the samples was checked again and the final dissolved Am concentrations were determined after ultrafiltration (10 kDa) to exclude the contribution of colloidal particles. In the pH range of 8-9, which is relevant to the KURT-DB3 groundwater condition, the measured dissolved Am(III) concentrations were converged to around 10-8 M. These values are higher than the solubility of AmCO3OH:0.5H2O(s), but lower than that of AmCO3OH(am). There was no indication of transformation of the amorphous phase to the crystalline phase in our observation time window.
Dissolution behaviors of ThO2(cr) and PuO2(cr) in synthetic groundwater were investigated at room temperature (23 2°C) under atmospheric conditions. The synthetic groundwater was prepared according to the chemical composition of the KURT-DB3 groundwater. The pH and Eh of the synthetic groundwater were pH 8.9 and 0.5 V, respectively, and the major components were Na, K, Ca, Mg, Si, Cl, SO4, F and HCO3 ions. A few mg of ThO2(cr) and PuO2(cr) powder were added in the synthetic groundwater and the concentrations of Th and Pu in supernatant were monitored for 5 months of reaction time. The concentrations of Th before and after ultracentrifugation were compared, while the solid-liquid phase separation of Pu samples could not be applied due to the small volume of sample solutions. The concentrations of Th and Pu were measured by ICP-MS and alpha spectrometry, respectively. Geochemist’s Work Bench (GWB, standard, 17.0) was applied for the modeling with ThermoChimie TDB v. 11a, which was updated with the latest NEA-TDB (vol. 14). Aqueous species distributions and solubility limiting solid phases of Th and Pu under the synthetic groundwater conditions were evaluated. The results of geochemical modeling indicate that aqueous Th-OH-CO3 ternary species and Pu(IV) species are dominant in solutions equilibrated with ThO2(s) and PuO2(am, hyd), respectively. The dissolution behaviors of ThO2(cr) and PuO2(cr) are comparable to the dissolution of ThO2(aged, logKsp = 8.5) and the oxidative dissolution of PuO2(am, hyd) in the presence of PuO2(coll, hyd), respectively.
Two sets of analyses for the cases of groundwater release to well and sea ecosystems were conducted for the environmental impact assessment of high-level radioactive waste disposal facilities. After obtaining the respective BDCF (Biosphere Dose Conversion Factor) results for the scenarios of well-farming and marine water fishing using different biosphere assessment conceptual models implemented in ECOLEGO, they were compared each other. The purposes of these analyses are to identify reference generic biosphere conceptual models and to get insight on model uncertainty. In this study, the endpoint used for the comparison of the ECOLEGO biosphere models was the socalled Biosphere Dose Conversion Factor (BDCF), which is defined as the maximum value of the total dose to the exposed group, in Sv/yr, resulting from a continuous unit release of 1 Bq/yr during the whole simulation time either to the well compartment (BDCF_Well) or to the marine water compartment (BDCF_Sea). The radionuclides considered in the comparison were Cs-137, I-129, Nb-94, Ni-59, Ni- 63, Sr-90 and Tc-99. The conceptual models used in the biosphere assessment of the releases to a well are based on models that have been used by the DOE (simple-soil model) and SKB (complex-soil model) in safety assessments of radioactive waste repositories, respectively. Difference between two conceptual models used in the assessment of the releases to a sea is the number of compartments representing the sea; i.e., one model represents the sea with one compartment for the water and one for the sediment (singlecompartment model), whereas the alternative model uses two compartments for the water and the sediments: one for the inner coast and one for the outer coast (double-compartment model). The results of the BDCF_Well to a farmer obtained with the DOE and SKB models are shown to be very close to each other. Despite the differences in conceptual models and parameters, the results are within a maximum difference of a factor of 4. The results from the SKB model were higher for all radionuclides. The values of the BDCF_Sea obtained with the single- and double-compartment models are shown to be larger differences with a maximum order of 2. For all studied radionuclides, the double-compartment model produces higher BDCFs than does the single-compartment model. The differences would be due to activity concentrations in both water and sediments. Since the hydrodynamic behavior assumed for flow in the sea could significantly influence the dilution volumes and hence the concentrations, it is found that site-specific investigations are necessary to establish an appropriate marine biosphere conceptual model.