Sugiura, Yuki; Ishidera, Takamitsu; Tachi, Yukio
Applied Clay Science, 200, p.105910_1 - 105910_10, 2021/01
Okubo, Takahiro*; Yamazaki, Akio*; Fukatsu, Yuta; Tachi, Yukio
Microporous and Mesoporous Materials, 313, p.110841_1 - 110841_11, 2021/01
Pore distributions in water-saturated Ca-montmorillonite were investigated using H NMR measurements under various dry densities (0.8 - 1.6 g/cm) and porewater salinity conditions (deionized water, 0.1 and 1 M CaCl), at the temperature range of 233 - 303 K. The volume fractions of the interlayer pore including two and three hydrated layers and the non-interlayer pore in compacted Ca-montmorillonite were quantified by NMR relaxometry including and distribution analysis, and were compared with NMR cryoporometry and X-ray diffractometry. These analysis provided consistent pictures on the pore distributions in compacted Ca-montmorillonite, in contrast to Na-montmorillonite. The main factor affecting the pore distribution in compacted Ca- and Na-montmorillonite is the density, whereas the effect of porewater salinity is relatively smaller. The effect of interlayer cations is also relatively smaller at higher density, although the differences in the pore structures are significant at low density.
Francisco, P. C. M.; Tachi, Yukio
ACS Earth and Space Chemistry (Internet), 4(12), p.2366 - 2377, 2020/12
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
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.
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
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.
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
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.
Sugiura, Yuki; Tomura, Tsutomu*; Ishidera, Takamitsu; Doi, Reisuke; Francisco, P. C. M.; Shiwaku, Hideaki; Kobayashi, Toru; Matsumura, Daiju; Takahashi, Yoshio*; Tachi, Yukio
Journal of Radioanalytical and Nuclear Chemistry, 324(2), p.615 - 622, 2020/05
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) setting and development of mechanistic sorption models. K 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 setting and development of mechanistic models, i.e., clay minerals, sedimentary rocks and cementitious materials. As a result, 6,702 K data from 60 references were added and the total number of K values in JAEA-SDB reached 69,679. The QA/classified K data reached about 72% for all K data in JAEA-SDB.
Tachi, Yukio; Suyama, Tadahiro*; Mihara, Morihiro
JAEA-Data/Code 2019-021, 101 Pages, 2020/03
Sorption of radionuclides in cement and bentonite as engineered barrier materials, and rocks as natural barrier is the one of key processes in the performance assessment of geological disposal of TRU and high-level waste. The magnitude of sorption, expressed normally by a distribution coefficient (K), needs to be measured and determined taking into account the properties of barrier materials and geochemical conditions and associated uncertainty in the performance assessment. The basic concept for TRU waste disposal contains cementitious materials as an engineered barrier materials, in addition to bentonite and rock. It is therefore needed to consider the effects of the cement degradation and co-existing substances such as nitrates on radionuclide sorption. This report focused on data acquisition of distribution coefficient (K) by batch sorption experiments for the systems coupling barrier material-chemical condition-radionuclides that are needed to consider for the performance assessment of geological disposal of TRU waste. The barrier materials considered are ordinary Portland cement (OPC), degraded OPC and tuff rock. The chemical conditions are distilled water and synthetic seawater equilibrated with OPC and those containing nitrates and ammonium salts, etc. The radionuclides considered are organic carbon, inorganic carbon, Cl, I, Cs, Ni, Se, Sr, Sn, Nb, Am and Th. Although K values have been partly reported previously as RAMDA (Radionuclide Migration Datasets) for the performance assessment in the TRU-2 report, these results and addition K data are reported with the details of experimental methods and conditions.
Francisco, P. C. M.; Mitsui, Seiichiro; Ishidera, Takamitsu; Tachi, Yukio; Doi, Reisuke; Shiwaku, Hideaki
Geochimica et Cosmochimica Acta, 270, p.1 - 20, 2020/02
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
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 140C, 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 60C to that for illite + quartz at higher temperatures. However, even over very long timescales ( 1 Ma), smectite does not transform to illite under thermodynamically-favourable conditions at temperatures less than 80C.
Hamamoto, Takafumi*; Ishida, Keisuke*; Shibutani, Sanae*; Fujisaki, Kiyoshi*; Tachi, Yukio; Ishiguro, Katsuhiko*; McKinley, I. G.*
Proceedings of 2019 International High-Level Radioactive Waste Management Conference (IHLRWM 2019) (USB Flash Drive), p.77 - 82, 2019/04
Takahashi, Hiroaki*; Tachi, Yukio
Applied Clay Science, 168, p.211 - 222, 2019/02
Microstructural and mass transport properties of compacted Na- and Cs-montmorillonites with different swelling properties were investigated by combining 3D microstructure analysis using nanofocus X-ray CT and diffusion measurement of HDO. The X-ray CT observations indicated that macropores in the dry state of compacted Na-montmorillonite are filled with gel phases, and the grain sizes of clay particles shifted toward smaller values through the saturation and swelling processes. By contrast, no gel phase and no decrease in the grain and pore volumes were observed for saturated Cs-montmorillonite. The geometrical factors of the macropores including tortuosity and geometric constrictivity of saturated Cs-montmorillonite determined by the X-ray CT was consistent with the corresponding values derived in the HDO diffusion test. In the case of Na-montmorillonite, the larger differences between the geometric factors evaluated by the X-ray CT and the diffusion tests can be explained by the electrostatic constrictivity factor and the additional geometrical factors in gel phase and interlayer that are smaller than the detection limit of the X-ray CT.
Soler, J. M.*; Neretnieks, I.*; Moreno, L.*; Liu, L.*; Meng, S.*; Svensson, U.*; Trinchero, P.*; Iraola, A.*; Ebrahimi, H.*; Molinero, J.*; et al.
SKB R-17-10, 153 Pages, 2019/01
The SKB Task Force is an international forum on modeling of groundwater flow and solute transport in fractured rock. The WPDE experiments are matrix diffusion experiments in gneiss performed at the ONKALO underground facility in Finland. Synthetic groundwater containing several conservative and sorbing tracers was injected along a borehole interval. The objective of Task 9A was the predictive modeling of the tracer breakthrough curves from the WPDE experiments. Several teams, using different modelling approaches, participated in this exercise. An important conclusion from this exercise is that the modeling results were very sensitive to the magnitude of dispersion in the borehole opening, which is related to the flow of water. Focusing on the tails of the breakthrough curves, which are more directly related to matrix diffusion and sorption, the results from the different teams were more comparable. The modeling results have also been finally compared to the measured breakthroughs.
Yotsuji, Kenji*; Tachi, Yukio; Kawamura, Katsuyuki*; Arima, Tatsumi*; Sakuma, Hiroshi*
Nendo Kagaku, 58(1), p.8 - 25, 2019/00
Molecular dynamics (MD) simulations were conducted to investigate physical properties of water and cations in montmorillonite interlayer nanopores. The swelling behaviors and hydration states were firstly evaluated as functions of interlayer cations and layer charge. The diffusion coefficients of water and cations in interlayer nanopores were decreased in comparison with those in bulk water and came closer to those in bulk water when basal spacing increased. The viscosity coefficients of interlayer water estimated indicated a significant effect of viscoelectricity at 1- and 2-layer hydration states and higher layer charge of montmorillonite. These trends from MD calculations were confirmed to be consistent with existing measured data and previous MD simulation. In addition, model and parameter related to viscoelectric effect used in the diffusion model was refined based on comparative discussion between MD simulations and measurements. The series of MD calculations could provide atomic level understanding for the developments and improvements of the diffusion model for compacted montmorillonite.
Okubo, Takahiro*; Okamoto, Takuya*; Kawamura, Katsuyuki*; Gugan, R.*; Deguchi, Kenzo*; Oki, Shinobu*; Shimizu, Tadashi*; Tachi, Yukio; Iwadate, Yasuhiko*
Journal of Physical Chemistry A, 122(48), p.9326 - 9337, 2018/12
The structures of Cs adsorption on montmorillonite were investigated by the nuclear magnetic resonance (NMR) spectroscopy. The NMR spectra of Cs adsorbed on montmorillonite samples were measured under different Cs contents and relative humidity levels. NMR parameters were evaluated by the first principle calculations in order to identify the relationship between adsorbed Cs structures and NMR parameters. The comparisons between experimental and theoretical NMR spectra revealed that Cs is preferentially adsorbed at sites near Al for low Cs substituted montmorillonites, and that non-hydrated Cs present in partially Cs substituted samples, even after being hydrated under high relative humidity.
Ishidera, Takamitsu; Tachi, Yukio; Akagi, Yosuke*; Ashida, Takashi
Progress in Nuclear Science and Technology (Internet), 5, p.221 - 224, 2018/11
In Fukushima Daiichi Nuclear Power Station, radionuclides are removed from contaminated water by the decontamination system using zeolite. In this study, sorption properties of U and Np on zeolite were investigated by batch sorption experiments to obtain fundamental information for predicting the radionuclides inventory. High distribution coefficients were observed for U in the simulated sea water diluted 10 times by deionized water. In contrast, low distribution coefficient of U was observed in simulated sea water. Low distribution coefficients were observed for Np independent of simulated sea water concentration. Batch sorption experiments of U carried out as functions of sodium ion and total inorganic carbon concentration suggested that the distribution coefficient of U was strongly affected by the total inorganic carbon concentration. This result suggests that aqueous species of radionuclides and their sorption behavior need to be considered to estimate the inventory of radionuclides in zeolite.
Tachi, Yukio; Ochs, M.*
Progress in Nuclear Science and Technology (Internet), 5, p.229 - 232, 2018/11
Various types of post-accident radioactive waste have been generated from cleanup and decommissioning activities at the Fukushima Daiichi Nuclear Power Plant. For the disposal of these wastes, perturbation effects resulting from co-existing substances (e.g., organic substances, boron, and salts) are needed to be considered. Such co-existing substances may influence on the radionuclide sorption parameters for the safety assessment of the disposal systems. The present study focuses on developing the methodology to quantify sorption parameters by considering such perturbation effects and illustrating example calculations regarding the sorption reduction factors (SRFs) due to the presence of organic ligands (ISA) for cement systems. Three approaches for the derivations of SRFs for cement-Am-ISA case were compared. These options should be applied as a stepwise manner according to the data availability for the perturbation effects resulting from the co-existing substances.
Ochs, M.*; Vriens, B.*; Tachi, Yukio
Progress in Nuclear Science and Technology (Internet), 5, p.208 - 212, 2018/11
The clean-up activities related to the accident at the Fukushima Nuclear Power Plant give rise to several types of wastes containing cementitious materials, such as concrete. Further, the use of cement-based barriers may be considered, due to their favorable and stable chemical properties, including their ability to sorb or incorporate radionuclides. Wastes from Fukushima are expected to contain substances that can have perturbing effects on retention, especially organic complexing substances, boron, and chloride salts. The present study focuses on a methodology for quantifying the retention behaviour of UVI) and U(IV) in cement materials of different degradation and in the presence of organics, boron, and salts on the basis of available literature information. A stepwise approach is proposed and illustrated for Kd setting for U(VI) and U(IV).
Akagi, Yosuke*; Kato, Hiroyasu*; Tachi, Yukio; Sakamoto, Hiroyuki*
Progress in Nuclear Science and Technology (Internet), 5, p.233 - 236, 2018/11
A large amount of radioactive contaminated concrete will be generated from the decommissioning in the Fukushima Dai-ichi Nuclear Power Plant (NPP). For developing the plans of decommissioning and waste management including decontamination and disposal, it is important to estimate radionuclides inventory and concentration distribution in the concrete materials. In this study, effective diffusivities (De) and distribution coefficients (Kd) of HTO, Cs, I and U in OPC mortar were measured by through-diffusion and batch sorption experiments. De values derived were in the sequence of HTO, I, Cs, U, implying that cation exclusion effects may be important mechanisms in OPC mortar. Kd values derived by batch tests were higher by more than one order of magnitude than the diffusion-derived Kd values, indicating that crushing of samples had a strong influence on sorption. Diffusion and sorption mechanisms in OPC mortar were evaluated to predict the penetration behavior of these radionuclides.