• Nuclear Engineering and Technology
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• v.55 no.4
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• pp.1495-1506
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• 2023

For the safe disposal of high-level radioactive waste using Engineered Barrier Systems (EBS), bentonite buffer is used by its high swelling capability and low hydraulic conductivity. When the bentonite buffer is contacted to heated pore water containing ions by radioactive decay, chemical alterations of minerals such as illitization reaction occur. Illitization of bentonite indicates the alteration of expandable smectite into non-expandable illite, which threatens the stability and integrity of EBS. This study intends to provide a thorough review on the information underlying in the illitization of bentonite, by covering basic clay mineralogy, smectite expansion, mechanisms and observation of illitization, and illitization in EBS. Since understanding of smectite illitization is crucial for securing the safety and integrity of nuclear waste disposal systems using bentonite buffer, this thorough review study is expected to provide essential and concise information for the preventive EBS design.

• Korean Journal of Mineralogy and Petrology
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• v.36 no.1
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• pp.41-54
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• 2023

Illite is a common mineral that forms readily from feldspar and mica via hydrothermal alteration and exhibits various characteristics depending on the degree of hydrothermal alteration. To ensure continued mining of high-quality illite ore, it is crucial to understand the illitization. Thus, this study collected ores from two illite ore deposit and their surrounding alteration zones in Yeongdong-gun, Chungcheongbuk-do, a significant source of illite in the Republic of Korea, to determine the constituent mineral contents and textural characteristics. Polarized light microscopy analyses revealed that the illite ore deposit were highly illitized with little remaining textural characteristics of the parent mica schist, and only some quartz was present. The ore zone contained illite, muscovite, quartz, and feldspar, with illitization primarily occurring around feldspar and quartz. X-ray diffraction analyses identified that the content of illite/muscovite was approximately 50-75 wt.%, with a maximum of 75 wt.%. Additionally, X-ray fluorescence analyses indicated a linear increase in K₂O content with increasing illite content, showing the highest correlation among the major components analyzed. It is suggested that the illite in the Yeongdong area results from feldspar and quartz alteration by hydrothermal fluids along the fault, with illitization of feldspar occurring before that of quartz. The results of this study are expected to contribute to the development of high-quality illite ore deposit in Yeongdong, Chungcheongbuk-do.

• Proceedings of the Petrological Society of Korea Conference
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• 2000.05a
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• pp.93-96
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• 2000

• Journal of Soil and Groundwater Environment
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• v.26 no.5
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• pp.29-38
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• 2021

This study investigated the mineralogical properties of bentonite and illite and evaluated the Cs sorption at various concentrations (C_w≈1-10⁵ ㎍/L). Bentonite samples, collected from South Korea and USA, majorly consisted of Ca- and Na-montmorillonite, showed large cation exchange capacity (CEC, 91.4 and 47.3 meq/100 g) and specific surface area (SSA, 46.1 and 39.7 m²/g). In contrast, illite sample (USA) had relatively low values for 14.4 meq/100g of CEC and 29.3 m²/g of SSA, respectively. Bentonite and illite had different non-linear sorption for Cs along with C_w. At low C_w<10 ㎍/L, illite showed higher sorption capacity than bentonite despite low CEC because of the existence of specific sorption sites at the weathered mineral edge. However, as C_w increased, bentonite represented high sorption capacity because the cation exchange between Cs and interlayer cations was effective at high C_w conditions. These results implicated that the Cs concentration is important to evaluate the sorption performance of bentonite and illite. Finally, the Cuadros' kinetic model for illitization using various K concentrations (2×10^-5 and 1.7×10^-3 mol/L) and temperature (100-200℃) showed that up to 50% of the montmorillonite in bentonite could be converted to illite, suggesting that the illitization should be considered to evaluate the sorption performance of the bentonite in deep geological disposal repository.

• Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT)
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• v.19 no.4
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• pp.459-467
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• 2021

In the majority of countries, the upper limit of buffer temperature in a repository is set to below 100℃ due to the possible illitization. This smectite-to-illite transformation is expected to be detrimental to the swelling functions of the buffer. However, if the upper limit is increased while preventing illitization, the disposal density and cost-effectiveness for the repository will dramatically increase. Thus, understanding the characteristics and creating a database related to the buffer under the elevated temperature conditions is crucial. In this study, a strategy to investigate the bentonite found in Korea under the elevated temperatures from a mineral transformation and radionuclides retardation perspective was proposed. Certain long-term hydrothermal reactions generated the bentonite samples that were utilized for the investigation of their mineral transformation and radionuclide retardation characteristics. The bentonite samples are expected to be studied using in-situ synchrotron-based X-Ray Diffraction (XRD) technique to determine the smectite-to-illite transformation. Simultaneously, the 'high-temperature and high-pressure mineral alteration measurement system' based on the Diamond Anvil Cell (DAC) will control and provide the elevated temperature and pressure conditions during the measurements. The kinetic models, including the Huang and Cuadros model, are expected to predict the time and manner in which the illitization will become detrimental to the performance and safety of the repository. The sorption reactions planned for the bentonite samples to evaluate the effects on retardation will provide the information required to expand the current knowledge of repository optimization.

• Journal of Nuclear Fuel Cycle and Waste Technology(JNFCWT)
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• v.13 no.4
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• pp.283-293
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• 2015

The buffer is a key component of the engineered barrier system in a high-level radioactive waste (HLW) repository. The present study reviewed the requirements and functional criteria of the buffer reported in literature, and also based on the results, proposed an approach to establish a buffer concept which is applicable to an HLW repository in Korea. The hydraulic conductivity, radionuclide-retarding capacity (equilibrium distribution coefficient and diffusion coefficient), swelling pressure, thermal conductivity, mechanical properties, organic carbon content, and illitization rate were considered as major technical parameters for the functional criteria of the buffer. Domestic bentonite (Ca-bentonite) and, as an alternative, MX-80 (Na-bentonite) were proposed for the buffer of an HLW repository in Korea. The technical specifications for those proposed bentonites were set to parameter values that conservatively satisfy Korea's functional criteria for the Ca-bentonite and Swedish criteria for the Na-bentonite. The thickness of the buffer was determined by evaluating the means of shear behavior, radionuclide release, and heat conduction, which resulted in the proper buffer thickness of 0.25 to 0.5 m. However, the final thickness of the buffer should be determined by considering coupled thermal-hydraulic-mechanical evaluation and economics and engineering aspects as well.

• Economic and Environmental Geology
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• v.42 no.5
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• pp.395-401
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• 2009

The smectite-illite (SI) reaction is a ubiquitous process in siliciclastic sedimentary environments. For the last 4 decades the importance of smectite to illite (S-I) reaction was described in research papers and reports, as the degree of the (S-I) reaction, termed "smectite illitization", is linked to the exploration of hydrocarbons, and geochemical/petrophysical indicators. The S-I transformation has been thought that the reaction, explained either by layer-by-layer mechanism in the solid state or dissolution/reprecipitation process, was entirely abiotic and to require burial, heat, and time to proceed, however few studies have taken into account the bacterial activity. Recent laboratory studies showed evidence suggesting that the structural ferric iron (Fe(III)) in clay minerals can be reduced by microbial activity and the role of microorganisms is to link organic matter oxidation to metal reduction, resulting in the S-I transformation. In abiotic systems, elevated temperatures are typically used in laboratory experiments to accelerate the smectite to illite reaction in order to compensate for a long geological time in nature. However, in biotic systems, bacteria may catalyze the reaction and elevated temperature or prolonged time may not be necessary. Despite the important role of microbe in S-I reaction, factors that control the reaction mechanism are not clearly addressed yet. This paper, therefore, overviews the current status of microbially mediated smectite-to-illite reaction studies and characterization techniques.

• Economic and Environmental Geology
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• v.34 no.3
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• pp.243-254
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• 2001

Variation in relative contents of clay minerals was used to genetically interpret depositional environment of the Upper Jurassic Solnhofen limestone. Mineralogical examination of whole rocks and clay fractions indicates that the faule and flinz beds are composed mainly of calcite and quartz with minor amount of clay minerals such as illite, kaolinite, and smectite. Smectite shows a trend of illitization: illite layers increase with increasing of burial depth. With increasing burial depth, relative abundance of kaolinite with quartz and illite increases. This implies that the Solnhofen basin was formed during the transgression based on reduce of terrigenous influx.

• Nuclear Engineering and Technology
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• v.53 no.5
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• pp.1511-1518
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• 2021

In most countries, the thermal criteria for the engineered barrier system (EBS) is set to below 100 ℃ due to the possible illitization in the buffer, which will likely be detrimental to the performance and safety of the repository. On the other hand, if the thermal criteria for the EBS increases, the disposal density and the cost-effectiveness for the high-level radioactive wastes will dramatically increase. Thus, fundamentals on the thermal behavior of the buffer under the elevated temperatures is of crucial importance. Yet, the behaviors at the elevated temperatures of the bentonite under groundwater-saturated conditions have not been reported to-date. Here, we have developed an in-situ synchrotron-based method for the thermal behavior study of the buffer under the elevated temperatures (25-250 ℃), investigated dspacings of the montmorillonite in the Korean bentonite (i.e., Ca-type) at dry and KURT (KAERI Underground Research Tunnel) groundwater-saturated conditions (KJ-ii-dry and KJ-ii-wet), and compared the behaviors with that of MX-80 (i.e., Na-type, MX-80-wet). The hydration states analyzed show tri-, bi-, and mono-hydrated at 25, 120, and 250 ℃, respectively for KJ-ii-wet, whereas tri-, mono-, and de-hydrated at 25, 150, and 250 ℃, respectively for MX-80-wet. The Korean bentonite starts losing the interlayered water at lower temperatures; however, holds them better at higher temperatures as compared with MX-80.

• Economic and Environmental Geology
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• v.28 no.4
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• pp.327-335
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• 1995

Illite/smectite (I/S) in the Beaufort-Mackenzie Basin, Arctic Canada has been scrutinized on the basis of mineralogical analysis of 215 core and drill-cutting samples from 22 exploratory wells onshore and offshore. I/S in the Beaufort-Mackenzie Basin includes the following four types: random, a mixture of random and ordered, R1-ordered, and R>1-ordered I/S. A mixture of random and ordered I/S occurs in the transitional interval between random and R>1-ordered I/S, and may represent a metastable state in the ordering reaction. A widespread occurrence of the mixture in natural environments suggests that the ordering reaction may be a slow process that results in co-existence of reactants and products. K-saturation experiments show that layer charges of expandable layers in I/S are variable. High-charge expandable layers transform into illite-like layers upon simple K-saturation. K-saturation alters the composition and/or the degree of ordering in I/S, suggesting that illitization in nature can be transformational.