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Journal Articles

The Impact of cement on argillaceous rocks in radioactive waste disposal systems; A Review focusing on key processes and remaining issues

Wilson, J.*; Bateman, K.; Tachi, Yukio

Applied Geochemistry, 130, p.104979_1 - 104979_19, 2021/07

 Times Cited Count:1 Percentile:0.56(Geochemistry & Geophysics)

The concept of deep geological disposal will include the multiple use of cement-based materials. In the case of argillaceous host rocks, the presence of hyperalkaline cement porefluid results in the destabilization of primary minerals in the argillite, resulting in the development of a zone of alteration at cement-rock interfaces. The process understanding gained from experimental, analogue, and modelling studies has been reviewed, and remaining areas of uncertainty identified. Although there is a reasonably good understanding of the mineral assemblages that are likely to occur due to cement-rock interactions, there are still some areas where a degree of uncertainty remains, in particular: the evolution of cement-argillite interfaces at T $$>$$ 25$$^{circ}$$C; the rates at which secondary minerals form; the extent of pore clogging due to secondary mineral precipitation; the implications of alteration for radionuclide transport.

Journal Articles

Consideration on modeling of Nb sorption onto clay minerals

Yamaguchi, Tetsuji; Ohira, Saki; Hemmi, Ko; Barr, L.; Shimada, Asako; Maeda, Toshikatsu; Iida, Yoshihisa

Radiochimica Acta, 108(11), p.873 - 877, 2020/11

 Times Cited Count:0 Percentile:0.01(Chemistry, Inorganic & Nuclear)

Journal Articles

Using natural systems evidence to test models of transformation of montmorillonite

Savage, D.*; Wilson, J.*; Benbow, S.*; Sasamoto, Hiroshi; Oda, Chie; Walker, C.*; Kawama, Daisuke*; Tachi, Yukio

Applied Clay Science, 195, p.105741_1 - 105741_11, 2020/09

 Times Cited Count:1 Percentile:0.02(Chemistry, Physical)

Safety functions for the clay buffer in a repository for high-level radioactive waste (HLW) are fulfilled if the presence of montmorillonite with high swelling capacity and low permeability is maintained in the long-term. The transformation of montmorillonite to the non-swelling mineral likely illite is addressed in most safety assessments by using simple semi-empirical kinetic models, but this approach contrasts with more complex reactive-transport simulations. In the present study, reactive-transport simulations are compared with simple semi-empirical kinetic models. Results suggest that reactive-transport simulations err on the side of conservatism, but may produce unrealistic estimates of illitization. This comparison demonstrates that reactive-transport models may be carefully applied to simulate the long-term evolution of near field environment for HLW disposal.

Journal Articles

Key factors controlling radiocesium sorption and fixation in river sediments around the Fukushima Daiichi Nuclear Power Plant, 1; Insights from sediment properties and radiocesium distributions

Tachi, Yukio; Sato, Tomofumi*; Akagi, Yosuke*; Kawamura, Makoto*; Nakane, Hideji*; Terashima, Motoki; Fujiwara, Kenso; Iijima, Kazuki

Science of the Total Environment, 724, p.138098_1 - 138098_11, 2020/07

 Times Cited Count:5 Percentile:70.14(Environmental Sciences)

To understand and predict radiocesium transport behaviors in the environment, highly contaminated sediments from Ukedo and Odaka rivers around the Fukushima Daiichi Nuclear Power Plant were investigated systematically focusing on key factors controlling radiocesium sorption and fixation, including particle size, clay mineralogy and organic matter.

Journal Articles

Key factors controlling radiocesium sorption and fixation in river sediments around the Fukushima Daiichi Nuclear Power Plant, 2; Sorption and fixation behaviors and their relationship to sediment properties

Tachi, Yukio; Sato, Tomofumi*; Takeda, Chizuko*; Ishidera, Takamitsu; Fujiwara, Kenso; Iijima, Kazuki

Science of the Total Environment, 724, p.138097_1 - 138097_10, 2020/07

 Times Cited Count:2 Percentile:39.03(Environmental Sciences)

To understand and predict radiocesium transport behaviors in the environment, sorption and fixation behaviors of radiocesium on river sediments from Ukedo and Odaka rivers around the Fukushima Daiichi Nuclear Power Plant were investigated systematically focusing on Cs sorption and fixation mechanisms and their relationship with Cs concentrations and sediment properties including clay mineralogy and organic matter.

Journal Articles

Selective removal of radiocesium from micaceous clay for post-accident soil decontamination by temperature-controlled Mg-leaching in a column

Yin, X.; Zhang, L.*; Meng, C.*; Inaba, Yusuke*; Wang, X.*; Nitta, Ayako; Koma, Yoshikazu; Takeshita, Kenji*

Journal of Hazardous Materials, 387, p.121677_1 - 121677_10, 2020/04

JAEA Reports

Development of JAEA sorption database (JAEA-SDB); Update of sorption/QA data in FY2019

Sugiura, Yuki; Suyama, Tadahiro*; Tachi, Yukio

JAEA-Data/Code 2019-022, 40 Pages, 2020/03


Sorption behavior of radionuclides (RNs) in buffer materials, rocks and cementitious materials is one of the key processes in a safe geological disposal. This report focuses on updating of JAEA sorption database (JAEA-SDB) as a basis of integrated approach for the performance assessment (PA)-related distribution coefficient (K$$_{rm d}$$) setting and development of mechanistic sorption models. K$$_{rm d}$$ data and their quality assurance (QA) results were updated by focusing on the following systems as potential needs extracted from our recent activities on the K$$_{rm d}$$ setting and development of mechanistic models, i.e., clay minerals, sedimentary rocks and cementitious materials. As a result, 6,702 K$$_{rm d}$$ data from 60 references were added and the total number of K$$_{rm d}$$ values in JAEA-SDB reached 69,679. The QA/classified K$$_{rm d}$$ data reached about 72% for all K$$_{rm d}$$ data in JAEA-SDB.

JAEA Reports

Development of gel filler that facilitates fuel debris retrieval (Contract research); FY2018 Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development

Collaborative Laboratories for Advanced Decommissioning Science; Osaka University*

JAEA-Review 2019-029, 36 Pages, 2020/02


JAEA/CLADS, had been conducting the Center of World Intelligence Project for Nuclear Science/Technology and Human Resource Development (hereafter referred to "the Project") in FY2018. The Project aims to contribute to solving problems in nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2018, this report summarizes the research results of the "Development of Gel Filler that Facilitates Fuel Debris Retrieval". When gel materials such as polymer, silicate and clay minerals with adjusted viscosity are used in the process of debris retrieval, the gel would not leak down from the damaged parts, resulting in the reduction of surrounding air dose rate. In addition, gel materials can reduce the diffusion and scattering of dust that is produced by cutting. For these reasons, we propose a method where inside of a containment vessel is filled by gel materials in order to simplify the debris retrieval.

Journal Articles

Permeability measurement for macro-fractured granite using water including clay

Nara, Yoshitaka*; Kato, Masaji*; Sato, Tsutomu*; Kono, Masanori*; Sato, Toshinori

Proceedings of 5th ISRM Young Scholars' Symposium on Rock Mechanics and International Symposium on Rock Engineering for Innovative Future (YSRM 2019 and REIF 2019) (USB Flash Drive), 6 Pages, 2019/12

It is important to understand the long-term migration of radionuclides considering carious rock engineering projects such as the geological disposal of radioactive wastes. The network of fractures and pores in a rock mass can play important roles as the pathway of the fluid flow of rock. Usually groundwater contains fine-grained minerals such as clays. It is probable that the accumulation of the fine-grained minerals occurs in a fracture if the groundwater flows in a fracture in a rock. In this study, we have conducted the permeability measurement using water including clays. Specifically, we used a macro-fractured granite as a rock sample, and investigated the change of the permeability under the flow of the water including clays. It was shown that the hydraulic conductivity decreased with elapsed time.

Journal Articles

Natural systems evidence for the effects of temperature and the activity of aqueous silica upon montmorillonite stability in clay barriers for the disposal of radioactive wastes

Savage, D.*; Wilson, J.*; Benbow, S.*; Sasamoto, Hiroshi; Oda, Chie; Walker, C.*; Kawama, Daisuke*; Tachi, Yukio

Applied Clay Science, 179, p.105146_1 - 105146_10, 2019/10

 Times Cited Count:5 Percentile:57.36(Chemistry, Physical)

Natural systems evidence for the effects of temperature and the activity of aqueous silica upon montmorillonite stability was evaluated. Thermodynamic modeling using three different TDBs shows that stability fields for montmorillonite exist from 0 to 140$$^{circ}$$C, but at low values of silica activity, a stability field for illite replaces that for montmorillonite. Pore fluid chemical and mineralogical data for sediments from ODP sites from offshore Japan show a trend from montmorillonite + amorphous silica stability at temperatures up to 60$$^{circ}$$C to that for illite + quartz at higher temperatures. However, even over very long timescales ($$gg$$ 1 Ma), smectite does not transform to illite under thermodynamically-favourable conditions at temperatures less than 80$$^{circ}$$C.

Journal Articles

Characterization of mineralogical controls on ammonium concentrations in deep groundwaters of the Horonobe area, Hokkaido

Sasamoto, Hiroshi; Sato, Hisao*; Arthur, R. C.*

Journal of Geochemical Exploration, 188, p.318 - 325, 2018/05

 Times Cited Count:0 Percentile:0.01(Geochemistry & Geophysics)

Ammonium is potentially an important constituent of deep groundwater under reducing condition. The retention of cesium by sorption in geological formations may have an important role ensuring the long-term safety of high-level radioactive waste. Cesium sorption will be affected by competing effects due to dissolve cation likely ammonium in groundwater, however. In the present study, a possible reaction to control of ammonium in deep groundwater was evaluated based on the data selected in the Horonobe as a test case in Japan. Results of investigation of mineralogy, thermodynamic evaluation of groundwaters and the Electron Probe Micro Analysis (EPMA) to identify nitrogen distribution on minerals suggest that the clay minerals bearing potassium, particularly smectite, illite and interstratified illite/smectite, appear to control the ammonium concentration in groundwaters by ion exchange reactions. Additionally, the selected groundwaters in the Horonobe seem to resemble to the gas and oil fields groundwater in the screened dataset in Japan in terms of ammonium distribution.

Journal Articles

Application of transient pulse method to permeability measurement for clay

Kato, Masaji*; Nara, Yoshitaka*; Okazaki, Yuki*; Kono, Masanori*; Sato, Toshinori; Sato, Tsutomu*; Takahashi, Manabu*

Zairyo, 67(3), p.318 - 323, 2018/03

To ensure the safe geological disposal of radioactive wastes, it is important to determine the permeability of clays. The transient pulse test is suitable to apply to the low permeability materials, because it takes relatively short term to determine the permeability. Usually we increase the upstream pore pressure in the measurement with the transient pulse test. However, it is impossible to determine the permeability of clay in this procedure because of the increase of pore pressure. Therefore, the transient pulse test has never been applied to the determination of permeability of clays. In this study, we tried to apply the transient pulse test to a clay obtained in Mizunami Underground Research Laboratory to determine the permeability with decreasing the downstream pore pressure. It was clarified that the transient pulse test with decreasing downstream pore pressure is appropriate from the measurements of granite and sandstone. It was shown that the permeability of a clay was determined by the transient pulse test with decreasing the downstream pore pressure, which agreed with the permeability determined from the falling head test. The measurement time of the transient pulse test is much shorter than that of the falling head test. It is concluded that the transient pulse test is appropriate for the determination of the permeability of clays.

Journal Articles

Desorption behavior of Cs from clay minerals by thermal heating in a vacuum; Analyses by thermal desorption spectroscopy and synchrotron radiation X-ray photoelectron spectroscopy

Hirao, Norie; Shimoyama, Iwao; Baba, Yuji; Izumi, Toshinori; Okamoto, Yoshihiro; Yaita, Tsuyoshi; Suzuki, Shinichi

Bunseki Kagaku, 65(5), p.259 - 266, 2016/05

 Times Cited Count:4 Percentile:19.67(Chemistry, Analytical)

After the Fukushima nuclear plant accident, radiocesium was strongly fixed to clay minerals in the soil. Some dry methods with heating are being developed to remove radiocesium from the soil. In this work, we propose a new dry method that combines heat treatment in vacuum and molten salts to reduce the processing temperature in dry methods. Vermiculite saturated with non-radioactive Cs was heated in vacuum, and Cs contents in the vermiculite were compared before and after heating using X-ray photoelectron spectroscopy. Approximately 40% of cesium were removed by heating at 800$$^{circ}$$C for three minutes when only vermiculite was heated. Approximately 70% of cesium were removed by heating at 450$$^{circ}$$C for three minutes when vermiculite was heated with NaCl/CaCl$$_{2}$$ mixed salts. Based on these results, this method is expected to reduce temperature and increase efficiency on dry methods for cesium removal from clay minerals.

Journal Articles

Clay-based modeling approach to diffusion and sorption in the argillaceous rock from the Horonobe URL; Application to Ni(II), Am(III), and Se(IV)

Tachi, Yukio; Suyama, Tadahiro; Yotsuji, Kenji; Ishii, Yasuo; Takahashi, Hiroaki*

CMS Workshop Lectures, Vol.21, p.241 - 250, 2016/00

Sorption and diffusion of radionuclides in argillaceous rocks are key processes in the safe geological disposal. The diffusion and sorption behavior of Ni(II), Am(III) and Se(IV) in mudstone from the Horonobe URL were investigated by experimental and modeling approaches. Effective diffusivities obtained by the through-diffusion experiments were in the sequence of Cs$$^{+}$$, Ni$$^{2+}$$, HTO, I$$^{-}$$, Se(SeO$$_{4}$$$$^{2-}$$), Am(Am(CO$$_{3}$$)$$^{2-}$$) by comparison with the previous study. The distribution coefficient values were consistent with those obtained by batch sorption tests. These results were interpreted by the clay-based modeling approach coupling the thermodynamic sorption model assuming key contributions of clays (smectite and illite) and the diffusion model assuming the electrical double layer theory and the simplified pore model with size distribution. This clay-based model could provide reasonable account of observed trends and could be basically applicable for various radionuclides.

Journal Articles

Characterization of adsorbed alkali metal ions in 2:1 type clay minerals from first-principles metadynamics

Ikeda, Takashi; Suzuki, Shinichi; Yaita, Tsuyoshi

Journal of Physical Chemistry A, 119(30), p.8369 - 8375, 2015/07

 Times Cited Count:14 Percentile:59.87(Chemistry, Physical)

Adsorption states of alkali metal ions in three kinds of 2:1 type clay minerals are systematically investigated via first-principles-based metadynamics. Our reconstructed free energy surfaces in a two dimensional space of coordination numbers specifically employed as collective variables for describing the interlayer cations show that an inner-sphere (IS) complex is preferentially formed for Cs$$^{+}$$ in the 2:1 type trioctahedral clay minerals with saponitelike compositions, where lighter alkali ions show a tendency to form an outer-sphere one instead. The strong preference for an IS complex observed for Cs$$^{+}$$ is found to result partially from the capability of recognizing selectively Cs$$^{+}$$ ions at basal O atoms with the Lewis basicity significantly enhanced by the isomorphic substitution in tetrahedral sheets.

Journal Articles

Cesium-adsorption behavior of weathered biotite from Fukushima Prefecture depends on the degree of vermiculitization

Yamada, Hirohisa*; Yokoyama, Shingo*; Watanabe, Yujiro*; Suzuki, Masaya*; Suzuki, Shinichi; Hatta, Tamao*

Nihon Ion Kokan Gakkai-Shi, 25(4), p.207 - 211, 2014/11

JAEA Reports

Evaluation of soluble organic compounds generated by radiological degradation of asphalt

; Nishikawa, Yoshiaki*; ;

JNC TN8400 2001-002, 23 Pages, 2000/12


The soluble organic compounds generated by radiological degradation of asphalt ($$gamma$$ ray) were confirmed as a part of influence of the bituminized waste degradation in the TRU waste repositry. Especially, the influence of the nitrate was focused on. As a result, the concentration of the soluble organic compounds generated by radiological degradation of asphalt (10MGy, $$gamma$$ ray which is correspond to absorbed dose of asphalt for 1,000,000years) were lower (each formic acid : about 50mg/dm$$^{3}$$, acetic acid : about 30mg/dm$$^{3}$$ and oxalic acid : about 2mg/dm$$^{3}$$) than that of the formic acid, the acetic acid and the oxalic acid which Valcke et al. had shown (the influence of the organic at the solubility examination which uses Pu and Am). Moreover, the change in the concentration of TOC and the soluble organic compounds (formic acid, acetic acid and oxalic acid) is little under the existence of nitrate ion. That is, the formic acid and acetic acid which can be organic ligands were generated little by oxidative decomposition of asphalt in the process that nitrate ion becomes nitrite ion by radiation. The influence of the soluble organic compounds by the radiological degradation of the asphalt ($$gamma$$ ray) on adsorption and solubility by the complexation of radionuclides in the performance assessment can be limited.

JAEA Reports

Distribution coefficients of radionuclides in concrete waste for coastal soil and concrete powder

Kato, Shohei; Yanase, Yoshiaki

JAERI-M 93-113, 17 Pages, 1993/05


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