Effect of different interlayer counter-ions on montmorillonite swelling; Key controlling factors evaluated by molecular dynamic simulations

Yotsuji, Kenji*; Tachi, Yukio; Sakuma, Hiroshi*; Kawamura, Katsuyuki*

Genshiryoku Bakkuendo Kenkyu (CD-ROM), 29(2), p.63 - 81, 2022/12

https://doi.org/10.3327/jnuce.29.2_63

The understanding of the swelling phenomenon of montmorillonite is essential to predict the physical and chemical behavior of clay-based barriers in radioactive waste disposal systems. This study investigated the key factors controlling crystalline swelling behavior of montmorillonite with different interlayer counter-ions by molecular dynamics (MD) simulations. On the basis of the comparisons between MD simulated and experimental results, the water content in the interlayer in five homoionic (Na, K, Cs, Ca and Sr) montmorillonite was strongly correlated to the hydration number and the preference of an outer- or inner-sphere complex of each counter-ion. The detailed analysis for these results offer insights that the hydration number is controlled by the hydration free energy, the volume and the distribution of each interlayer counter-ion. The systematic MD simulations with virtually variable parameters clarified that the hydration free energy and the charge of interlayer counter- ions compete as influencing factors, and the control the formation rate of an outer-sphere complex of each counter-ion. The empirical relationships between these key factors will allow essential insights into predicting the swelling behavior of montmorillonite with different interlayer counter-ions.

Status of study of long-term assessment of transport of radioactive contaminants in the environment of Fukushima (FY2018) (Translated document)

Nagao, Fumiya; Niizato, Tadafumi; Sasaki, Yoshito; Ito, Satomi; Watanabe, Takayoshi; Dohi, Terumi; Nakanishi, Takahiro; Sakuma, Kazuyuki; Hagiwara, Hiroki; Funaki, Hironori; et al.

JAEA-Research 2020-007, 249 Pages, 2020/10

JAEA-Research-2020-007.pdf:15.83MB

The accident of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. occurred due to the Great East Japan Earthquake, Sanriku offshore earthquake, of 9.0 magnitude and the accompanying tsunami. As a result, large amount of radioactive materials was released into the environment. Under these circumstances, Japan Atomic Energy Agency (JAEA) has been conducting "Long-term Assessment of Transport of Radioactive Contaminants in the Environment of Fukushima" concerning radioactive materials released in environment, especially migration behavior of radioactive cesium since November 2012. This report is a summary of the research results that have been obtained in environmental dynamics research conducted by JAEA in Fukushima Prefecture.

Molecular dynamics simulations of physical properties of water and cations in montmorillonite interlayer; Application to diffusion model

Yotsuji, Kenji*; Tachi, Yukio; Kawamura, Katsuyuki*; Arima, Tatsumi*; Sakuma, Hiroshi*

Nendo Kagaku, 58(1), p.8 - 25, 2019/00

https://doi.org/10.11362/jcssjnendokagaku.58.1_8

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.

Stability of montmorillonite edge faces studied using first-principles calculations

Sakuma, Hiroshi*; Tachi, Yukio; Yotsuji, Kenji; Suehara, Shigeru*; Arima, Tatsumi*; Fujii, Naoki*; Kawamura, Katsuyuki*; Honda, Akira

Clays and Clay Minerals, 65(4), p.252 - 272, 2017/08

https://doi.org/10.1346/CCMN.2017.064062

Structure and stability of montmorillonite edge faces (110), (010), (100), and (130) of the layer charges y = 0.5 and 0.33 are investigated by the first-principles electronic calculations based on the density functional theory. Stacking and single layer models are tested for understanding the effect of stacking on the stability of montmorillonite edge faces. Most stacking layers stabilize the edge faces by making hydrogen bonds between the layers; therefore, the surface energy of stacking layers is reduced rather than the single layer model. This indicates that the surface energy of edge faces should be estimated depending on the swelling conditions. Lowest surface energies of (010) and (130) edge faces were realized by the presence of Mg ions on the edge faces. These edge faces have a strong adsorption site for cations due to local negative charge of the edges.

Redistribution and export of contaminated sediment within eastern Fukushima Prefecture due to typhoon flooding

Kitamura, Akihiro; Kurikami, Hiroshi; Sakuma, Kazuyuki; Malins, A.; Okumura, Masahiko; Machida, Masahiko; Mori, Koji*; Tada, Kazuhiro*; Tawara, Yasuhiro*; Kobayashi, Takamaru*; et al.

Earth Surface Processes and Landforms, 41(12), p.1708 - 1726, 2016/09

https://doi.org/10.1002/esp.3944

Sediment erosion and transport processes that are considered to be important in predicting the future radioactive material distribution through sediment-sorbed form in Fukushima Prefecture are simulated. Since large portion of the sediment is considered to be supplied into the rivers, it is important to trace their migration process in terms of each river basin. We choose five river basins, namely the Odaka, the Ukedo, the Maeda, the Kuma, and the Tomioka, from north to south, because of their importance in contamination aspects and prediction studies. The results are summarized as comprehensive dataset of sediment migration for particular river basins in typical typhoon events that account for the most of annual soil erosion. Detail calculations implemented for the amount of sediment supplied in to the river, deposited on river and dam beds, and exported to the ocean.

Radiation effects on MgAlO-yttria stabilized ZrO composite material irradiated with Ne ions at high temperatures

Hojo, Tomohiro*; Yamamoto, Hiroyuki; Aihara, Jun; Furuno, Shigemi*; Sawa, Kazuhiro; Sakuma, Takashi*; Hojo, Kiichi

Nuclear Instruments and Methods in Physics Research B, 250(1-2), p.123 - 127, 2006/09

https://doi.org/10.1016/j.nimb.2006.04.095

Spinel and yttria stabilized zirconia (YSZ) are candidates for fuel materials for use in nuclear reactors and the optical and insulating materials for fusion reactors. In the present study, the damage evolution process of polycrystalline spinel-YSZ composite materials has been studied by in situ transmission electron microscope observation during ion irradiation. The irradiation was performed with 30 keV Ne at a flux of 5 10 ions/cm per second at 923 K and 1473 K, respectively. At 923 K, defect clusters and bubbles were formed homogeneously in YSZ grains. On the other hand, at 1473 K, only bubble formation was observed. The bubbles grew remarkably with increasing ion fluence in both grains. Even though the growth of the bubbles was observed in both grains, the average diameter of grown bubbles in spinel grains was larger than those in YSZ ones. The bubbles tended to form along the grain boundary at both temperatures.

Ion beam surface modification of Y-TZP and effects of subsequent annealing

Motohashi, Yoshinobu*; Shibata, Taiju; Harjo, S.*; Sakuma, Takaaki*; Ishihara, Masahiro; Baba, Shinichi; Sawa, Kazuhiro

Proceedings of 14th International Federation for Heat Treatment and Surface Engineering Congress Transactions of Materials and Heat Treatment Vol.25 No.5, p.1032 - 1036, 2004/10

no abstracts in English

Variations in mechanical properties of zirconia-base ceramics due to superplastic deformations

Kikuchi, Makoto*; Motohashi, Yoshinobu*; Ito, Tsutomu*; Sakuma, Takaaki*; Shibata, Taiju; Baba, Shinichi; Ishihara, Masahiro; Sawa, Kazuhiro; Hojo, Tomohiro*; Tsuji, Nobumasa*

Nihon Kikai Gakkai Kanto Shibu Ibaraki Koenkai (2004) Koen Rombunshu (No.040-3), p.57 - 58, 2004/09

no abstracts in English

Radiation damage effects in superplastic 3Y-TZP irradiated with Zr ions

Motohashi, Yoshinobu*; Kobayashi, Tomokazu*; Harjo, S.*; Sakuma, Takaaki*; Shibata, Taiju; Ishihara, Masahiro; Baba, Shinichi; Hoshiya, Taiji

Nuclear Instruments and Methods in Physics Research B, 206, p.144 - 147, 2003/05

https://doi.org/10.1016/S0168-583X(03)00702-X

The 3mol% yttria containing tetragonal zirconia polycrystals(3Y-TZP) were irradiated using 130MeV Zr ions in the TANDEM accelerator facility at Tokai Research Establishment, JAERI. Irradiation was performed with the fluence of 3.510 and 2.110 ions/m. Residual stress and changes in mechanical properties caused by the ion irradiation and the effects of the subsequent annealing are studied. The occurrence of compressive residual stresses and increases in hardness and fracture toughness were found at the surface regions of as-irradiated specimens. It was found from the subsequent annealing that these quantities decreased gradually with raising the annealing temperature and returned to that of un-irradiated state at around 1173K. A most probable cause of the increases in the hardness and fracture toughness after the irradiation may, therefore, be the residual compressive stresses left in the irradiated surface region.

Ion irradiation effect on superplastic deformation behavior of ceramic material

Shibata, Taiju; Ishihara, Masahiro; Motohashi, Yoshinobu*; Baba, Shinichi; Hoshiya, Taiji; Sakuma, Takaaki*

Nihon Kikai Gakkai Kanto Shibu Ibaraki Koenkai (2002) Koen Rombunshu (No.020-3), p.123 - 124, 2002/09

Applications of superplastic ceramics to nuclear energy fields are very promising because of their superior mechanical and thermal properties. In this study, Zr ion irradiation effects on superplastic deformation behavior of a typical superplastic ceramic, 3mol% yttria containing tetragonal zirconia polycrystals (3Y-TZP), were studied. Zr ions with 130MeV were irradiated on the 3Y-TZP specimens by TANDEM accelerator at fluence levels of 3.5x10 and 2.1x10ions/m. Their mechanical properties were examined by three-point bending test at elevated temperatures after the irradiation. As a result, at the temperature range from the room temperature to 1473K, any obvious irradiation effects were not found by the bending test. On the other hand, at the range from 1623K to 1773K, it was found that the superplastic deformation behavior was changed by the Zr ion irradiation. The activation energy of superplastic deformation was increased with increasing the irradiation fluence.