Concerns with colloids, dispersed 1~1,000 nm particles, in the LILW repository are being raised due to their potential to enhance radionuclide release. Due to their large surface areas, radionuclides may sorb onto mobile colloids, and drift along with the colloidal transport, instead of being sorbed onto immobile surfaces. To prevent adverse implications on the safety of the repository, the colloidal impact must be evaluated. In this paper, colloid analysis done by SKB is studied, and factors to be considered for the safety assessment of colloids are analyzed. First, the colloid generation mechanism should be analyzed. In a cementitious repository, due to a highly alkaline environment, colloid formation from wastes may be promoted by the decomposition of organic materials, dissolution of inorganic materials, and corrosion of metals. Radiolysis is excluded when radionuclide inventory is moderate, as in the case of SKB. Second, colloid stability should be evaluated to determine whether colloids remain in dispersion. Stable colloids acquire electric charges, allowing particles to continuously repel one another to prevent coagulation. Thus, stability depends on the pH and ionic condition of the surroundings, and colloid composition. For instance, under a highly alkaline cementitious environment, colloids tend to be negatively charged, repelling each other, but Ca2+ ion from cement, acting as a coagulant, makes colloid unstable, promoting sedimentation. As in the case of SKB, the colloidal impact is assumed negligible in the silo, BMA, and BTF due to their extensive cement contents, but for BLA, with relatively less cement source, the colloidal impact is a potential concern. Third, colloid mobility should be assessed to appraise radionuclide release via colloid transport. The mobility depends on the density and size of colloids, and flow velocity to commence motion. As a part of the assessment, the filtration effect should also be included, which depends on pore size and structure. As in the case of SKB, due to static hydraulic conditions and engineering barriers, acting as efficient filters, colloidal transport is expected to be unlikely. In the domestic underground repository, the highly alkaline environment would lead to colloid formation, but due to high Ca2+ concentration and low flow velocity, colloids would achieve low stability and mobility, thus colloidal impact would be a minor concern. In the future, with further detailed analysis of each factor, waste composition, and disposal condition, reliable data for safety evaluation could be generated to be used as fundamental data for planning waste acceptance criteria.
In Korea, 483,102 assemblies of spent fuel have been discharged and stored in sites, as of 2019. However, total capacity for site storage is 529,748 assemblies, and more than 90% is already saturated. Wolsong site, the most saturated site, started to construct more dry storage to extend the capacity in 2020. Spent fuel and high-level waste (HLW) is a big concern in Korean nuclear industry. Then, master plan for management of spent fuel is once announced by Ministry of Trade, Industry and Energy (MOTIE) in 2016 and reviewed by civil committee in 2019. The core contents of the plan are establishing schedule for construction of HLW management facility in one area, and construction of temporary dry storage in each site, if unavoidable. For HLW management facility, there are three following schedules: siting of Underground Research Laboratory (URL) and Interim Storage by 2020, operation of facilities initiated by 2030, and operation of final disposal facility initiated by 2050. Final repository will be designed as deep geological repository. The concept of deep geological disposal is that spent nuclear fuel is placed in disposal containers that can withstand corrosion and pressure in long-term, permanently isolated from the human sphere of life, and dumped in deep geological media, such as crystalline rocks and clay layer, at a depth of 300 to 1,000 meters underground. The safety assessment of waste disposal sites focuses on determining whether the disposal sites meet the safety requirements of national regulatory authority. This safety assessment evaluates the potential radiation dose of radionuclides from the disposal site to humans or the environment. In this case, the calculation is performed assuming that all engineering barriers of the disposal site have collapsed in a long-term period. Then radionuclides are released from the waste, and migrated in groundwater. The dose resulting from the release and migration of radionuclides on the concentration of nuclides in groundwater. In general, metallic nuclides may exist in water in various ionic states, but some form colloids. This colloid allows more nuclides to exist in water than in solubility. Therefore, more doses may occur than we know generally predict. To determine the impact of colloids, we performed the safety assessment of the Yucca Mountain repository as an example.
According to the continued generation of spent nuclear fuel, a reliable safety assessment is highly required with the precise modeling of the migration and retardation behavior of radionuclides to enhance public acceptance and hinder excessive conservativeness during the construction of the repository. In particular, the colloids formed in the repository-relevant condition are known to accelerate the migration of radionuclides. Thus, geochemical behavior and relevant characteristics of colloids are needed to be unambiguously clarified. The objective of the present work is to investigate the fundamental characteristics of colloids contained in the natural groundwater system by using various analytical methods and the tangential flow ultra-filtration (TFUF) system. The granitic groundwater sample from the DB-3 borehole at the KURT (KAERI Underground Research Tunnel) was taken by an airtight stainless steel cylinder coated on the inside with PTFE to prevent the infiltration of ambient air into the geologic groundwater sample. And then, the groundwater sample was transferred to the inert glovebox filled with Ar gas to monitor the pH and Eh equilibrium of the aqueous sample. For further investigation, the colloid contained in the groundwater sample was concentrated by using the TFUF system equipped with a membrane filter (pore size: 3 kDa). The concentrated groundwater sample was analyzed with various methods such as ICP-MS/OES, IC, DLS/ELS, FE-TEM/SEM-EDS, ATR-FTIR, TOC, LC-OCD, etc. In this study, the size of groundwater colloids was determined to be 182.3 ± 52.7 nm with the major constituents of C, S, O, Fe, Al, Si, etc. The amount of organic carbon and the concentrations of organic substances determined by means of the molecular weight fraction with the TOC and LC-OCD provide further detailed information for the colloids in the KURT groundwater sample. The results obtained in this study are expected to be used as preliminary experimental data for modeling the colloid-facilitated migration of radionuclides to improve the reliability of the safety assessment of the geologic repository.
The fundamental characteristics of groundwater colloids, such as composition, concentration, size, and stability, were analyzed using granitic groundwater samples taken from the KAERI Underground Research Tunnel (KURT) site by such analytical methods as inductively coupled plasma-mass spectrometry, field emission-transmission electron microscopy, a liquid chromatography-organic carbon detector, and dynamic light scattering technique. The results show that the KURT groundwater colloids are mainly composed of clay minerals, calcite, metal (Fe) oxide, and organic matter. The size and concentration of the groundwater colloids were 10–250 nm and 33–64 μg·L−1, respectively. These values are similar to those from other studies performed in granitic groundwater. The groundwater colloids were found to be moderately stable under the groundwater conditions of the KURT site. Consequently, the groundwater colloids in the fractured granite system of the KURT site can form stable radiocolloids and increase the mobility of radionuclides if they associate with radionuclides released from a radioactive waste repository. The results provide basic data for evaluating the effects of groundwater colloids on radionuclide migration in fractured granite rock, which is necessary for the safety assessment of a high-level radioactive waste repository.
Colloid-facilitated migration has been significantly concerned with the acceleration of the radionuclide mobility in the HLW repository. In the repository system, the compacted bentonite, which is the buffer material, could be the major source for colloid generation; hence, the understanding of colloid generation from the bentonite is the essential to expect the colloid-facilitated radionuclide migration. This study aimed to investigate the colloid generation using a bentonite-based micro-scale flow path system, which called microfluidics. In order to fabricate the microfluidics, direct milling method was applied to make a mold by computer numerical control. The fabricated mold applied to prepare the microfluidic chip by Polydimethylsiloxane (PDMS), in which the size of microchannel was designed to be one micrometer. Initially, sylgard 184 and curing agent mixed and stirred for 10 min, afterwards the bubbles in the paste was removed in the vacuum desiccator for 30 min. Then the paste was poured into the mold, and finally dried for 4 hours at 80°C in a dry oven. The compacted Ca-bentonite chip was prepared by the cold isostatic pressing (CIP) method with the dry density of 1.6 g·cm−3. The microfluidic chip and compacted bentonite chip were assembled by an acryl jig, the flow rate was adjusted by 20 mL syringe equipped syringe pump. The degree of colloid generation accompanied with the erosion of bentonite was gravimetrically examined after the experiment. The effect of the pH and ionic strength on the colloid formation was investigated through the particle size, stability and aggregation. To the best of our knowledge, this is the first examination for the colloid generation using microfluidics; these results would give information to understand the colloid formation from the compacted Ca-bentonite in the HLW repository system.
본 연구에서는 국내산 경주벤토나이트를 이용하여 제조한 벤토나이트 콜로이드에 대한 산화환원 반응에 대체적으로 안정한 다가 핵종인 Eu(III)와 Th(IV)의 실험적 수착 연구를 수행하였다. 수착실험에 대한 공시험을 수행하여 반응용기 벽면에 의해, 침전에 의해, 콜로이드 형성에 의해 손실된 핵종들의 양을 평가하였다. 그리고 이러한 손실들을 반영한 Eu(III)와 Th(IV)의 벤토나이트 콜로이드에 대한 수착분배계수 값을 구하고 조사하였다. 세 종류의 손실양을 반영한 벤토나이트 콜로이드의 순수한 수착분배계수 값은 pH 변화에 따라 Eu(III)의 경우 정도의 값을 가지고, Th(IV)의 경우 정도의 값을 가지는 것으로 관측되었다. 특히 Eu(III)의 경우엔 pH 5 이상에서 침전의 영향이 크게 나타났고, Th(IV)의 경우엔 pH 3 이후에 콜로이드 형성과 침전의 영향이 크게 나타났다. 따라서 주어진 농도에서 콜로이드 형성 및 침전 영향이 커지는 pH 이후에는 Eu(III) 및 Th(IV)과 같은 다가 핵종들의 정확한 수착분배계수를 구하기 위해서는 이러한 침전 및 콜로이드 형성과 같은 영향이 반영되어야 할 것이다.
본 연구에서는 컬럼실험을 통해서 여러 종류의 콜로이드가 같이 존재할 때의 거동을 관찰하였다. 본 실험에서는 일반 pH조건에서 서로 반대의 표면전하를 띠는 ferrihydrite (100 nm; 양전하)와 비정질 SiO2 (40 nm, 80 nm; 음전하) 나노입자들와 음전하를 띠는 177~250μm의 석영을 고정상으로 이용하였다. 실험결과는, 양전하를 띠는 콜로이드(ferrihydrite)가 존재한다고 하더라도 그 비율이 많지 않으면 음전하를 띠는 콜로이드(SiO2)와의 상호작용에 의해서 석영고정상 속을 쉽게 이동될 수 있음을 보여주었다. 이는 자연조건하에서는 양전하를 띠는 오염물질과 음전하를 띠는 오염물질이 동시에 콜로이드에 의해서 이동될 수 있음을 지시한다.
강변여과는 강물을 강변의 충적대수층에 통과시켜 지층의 자체정화능력을 이용하여 오염물질을 상당량 저감시킨 후 양수하는 방식이다. 국내에서는 대부분의 원수를 지표수에서 취수하여 사용하고 있는 실정이나, 오염물질의 증가로 인하여 지표수를 원수로 사용하기가 점점 어려워지고 있다. 강변여과를 이용하여 양질의 원수를 확보하기 위해서는 오염물 이동에 관한 이해가 중요하다. 본 연구에서는 대수층에 용존성 유기물질(DOM)과 박테리아가 동시에 존재할 경우를 대상으로 대