Horiuchi, Yusuke; Watanabe, So; Sano, Yuichi; Takeuchi, Masayuki; Kida, Fukuka*; Arai, Tsuyoshi*
Journal of Radioanalytical and Nuclear Chemistry, 330(1), p.237 - 244, 2021/10
Applicability of tetra2-ehylhexyl diglycolamide (TEHDGA) impregnated adsorbent for minor actinide (MA) recovery from high level liquid waste (HLLW) in extraction chromatography technology was investigated through batch-wise adsorption and column separation experiments. Distribution ratio of representative fission product elements were obtained by the batch-wise experiments, and TEHDGA adsorbent was shown to be preferable to TODGA adsorbent for decontamination of several species. All Ln(III) supplied into the TEHDGA adsorbent packed column was properly eluted from the column, and the applicability of the adsorbent was successfully showed by this study.
Fujita, Yoshitaka; Seki, Misaki; Sano, Tadafumi*; Fujihara, Yasuyuki*; Kitagawa, Tomoya*; Matsukura, Minoru*; Hori, Junichi*; Suzuki, Tatsuya*; Tsuchiya, Kunihiko
Journal of Radioanalytical and Nuclear Chemistry, 327(3), p.1355 - 1363, 2021/03
We prepared three types of AlO with different surface structures and investigated Mo-adsorption/Tc-elution properties using [Mo]MoO that was irradiated in the Kyoto University Research Reactor. AlO adsorbed [Mo]molybdate ions in solutions at different pH; the lower was the pH, the higher was the Mo-adsorption capacity of AlO. The Tc-elution properties of molybdate ion adsorbed AlO were elucidated by flowing saline. Consequently, it was suggested that Mo-adsorption/desorption properties are affected by the specific surface of AlO and Tc-elution properties are affected by the crystal structure of AlO.
Takai, Shizuka; Kimura, Hideo*; Uchikoshi, Emiko*; Munakata, Masahiro; Takeda, Seiji
JAEA-Data/Code 2020-007, 174 Pages, 2020/09
The MIG2DF computer code is a computer program that simulates groundwater flow and radionuclide transport in porous media for the safety assessment of radioactive waste disposal. The original version of MIG2DF was released in 1992. The original code employs a two-dimensional (vertical or horizontal cross-section, or an axisymmetric configuration) finite-element method to approximate the governing equations for density-dependent saturated-unsaturated groundwater flow and radionuclide transport. Meanwhile, for geological disposal of radioactive wastes, landscape evolution such as uplift and erosion needs to be assessed as a long-term geological and climate events, considering site conditions. In coastal areas, the impact to groundwater flow by change of salinity distribution to sea level change also needs to be considered. To deal with these events in the assessment, we have revised the original version of MIG2DF and developed the external program which enables MIG2DF to consider unsteady landscape evolution. In these developments, this report describes an upgrade of MIG2DF (Version 2) and presents the configuration, equations, methods, and verification. This reports also give the explanation external programs of MIG2DF: PASS-TRAC (the particle tracking code), PASS-PRE (the code for dataset preparation), and PASS-POST (the post-processing visualization system).
Fujita, Yoshitaka; Seki, Misaki; Namekawa, Yoji*; Nishikata, Kaori; Kato, Yoshiaki; Sayato, Natsuki; Tsuchiya, Kunihiko; Sano, Tadafumi*; Fujihara, Yasuyuki*; Hori, Junichi*; et al.
KURNS Progress Report 2019, P. 157, 2020/08
no abstracts in English
Rizaal, M.; Saito, Takumi*; Okamoto, Koji*; Erkan, N.*; Nakajima, Kunihisa; Osaka, Masahiko
Mechanical Engineering Journal (Internet), 7(3), p.19-00563_1 - 19-00563_10, 2020/06
The adsorption of cesium (Cs) on calcium silicate insulation of primary piping system is postulated to contribute in high dose rate of surrounding pedestal area in Fukushima Daiichi NPP unit 2. In this study, room-temperature experiment of Cs adsorption on calcium silicate has been studied as an initial approach of Cs adsorption behavior toward higher temperature condition. As the result of analyzing of Cs adsorption kinetics, it was expected that the underlying adsorption mechanism is chemisorption. Furthermore, analysis of adsorption isotherm suggested unrestricted monolayer formation followed by multilayer formation.
Ota, Masakazu; Terada, Hiroaki; Hasegawa, Hidenao*; Kakiuchi, Hideki*
Science of the Total Environment, 704, p.135319_1 - 135319_15, 2020/02
Land-surface transfers of I are modeled and incorporated into a land-surface model (SOLVEG-II), and the model was applied to the observed transfer of I at a vegetated field impacted by atmospheric releases of I from Rokkasho reprocessing plant during 2007 to investigate the importance of each I-transfer pathway. The model calculation revealed that contamination of leaves of wild bamboo grasses was mostly caused by foliar adsorption of I (81%) induced via wet deposition of I. Wet deposition of I was the main I-input to the soil, ten-fold the dry deposition of I; however, the deposition of I during 2007 was only 2% of the model-assumed I that pre-existed in the soil; indicating the importance of long-term accumulation of I in soils. The model calculation also revealed that root uptake of I, not methylation, control the long-term turnover of soil I.
Fujita, Yoshitaka; Seki, Misaki; Namekawa, Yoji*; Nishikata, Kaori; Kimura, Akihiro; Shibata, Akira; Sayato, Natsuki; Tsuchiya, Kunihiko; Sano, Tadafumi*; Fujihara, Yasuyuki*; et al.
KURNS Progress Report 2018, P. 155, 2019/08
no abstracts in English
Nakajima, Kunihisa; Nishioka, Shunichiro; Suzuki, Eriko; Osaka, Masahiko
Proceedings of 27th International Conference on Nuclear Engineering (ICONE-27) (Internet), 8 Pages, 2019/05
Cesium chemisorption models were developed for estimation of amount of cesium chemisorbed onto stainless steel type 304 (SS304) during light water reactor severe accident. However, existing chemisorption models cannot accurately reproduce experimental results. In this study, a modified cesium chemisorption model was constructed based on a penetration theory for gas-liquid mass transfer with chemical reaction and was able to adequately describe effects on concentration of cesium hydroxide in gaseous phase and silicon content in SS304. It was found that the modified model can more accurately reproduce the experimental data than the existing model.
Suzuki, Eriko; Takase, Gaku; Nakajima, Kunihisa; Nishioka, Shunichiro; Hashimoto, Naoyuki*; Isobe, Shigehito*; Osaka, Masahiko
Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 4 Pages, 2019/05
In order to acquire the knowledge of the Cs chemisorption behaviour in the lower temperature region, the Cs chemisorbed compounds and the surface reaction rates were investigated by conducting the Cs chemisorption tests onto stainless steel at 873 and 973 K. As a result, The cesium ferrate compounds were revealed to be formed at this temperatures. It was seen that the dependences of surface reaction rate constant on this temperature were different from that at the higher temperature region. This behaviour leads to the conclusion that the Cs chemisorption model in the low temperature region should be newly constructed.
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.
Suzuki, Eriko; Nakajima, Kunihisa; Osaka, Masahiko
Progress in Nuclear Science and Technology (Internet), 5, p.165 - 167, 2018/11
In severe accident condition, CsFeSiO could be formed by Cesium (Cs) chemisorption onto reactor structural materials. For evaluation of re-vaporization behavior, effect of atmosphere on the vaporization behavior of CsFeSiO at high temperature was investigated by thermal gravimetric-differential thermal analyzer (TG-DTA) experiments. As a result, it was found that vaporization of CsFeSiO in reducing atmosphere (Ar-5%H) started at relatively low temperature, about 800C, compared with in atmosphere containing HO (Ar-5%H-5%HO). It was inferred that a possible chemical reaction for the weight loss at around 800C would occurred by the decomposition of CsFeSiO into volatile Cs vapor species under H.
Yu, Q.*; Tanaka, Kazuya; Kozai, Naofumi; Sakamoto, Fuminori; Tani, Yukinori*; Onuki, Toshihiko
ACS Earth and Space Chemistry (Internet), 2(8), p.797 - 810, 2018/08
Most of Mn oxides are biogenic and known to adsorb cesium (Cs) on the surface. This study investigated structural transformation of biogenic birnessite by accommodating commonly occurring natural heavy metals (Zn, Ni) during the formation of Mn oxides and the influence of those metals on the adsorption behavior of Cs on Mn oxides. It was found that the presence of heavy metals during bio-oxidation of Mn(II), followed by exposure to a low pH aqueous solution, increased the number of available layer vacancies, which consequently increased the adsorption capacity of Cs in the final product birnessite.
Kozai, Naofumi; Sakamoto, Fuminori; Tanaka, Kazuya; Onuki, Toshihiko; Sato, Takahiro*; Kamiya, Tomihiro*; Grambow, B.
Chemosphere, 196, p.135 - 144, 2018/04
Transformation of heavy elements by microbes such as bacteria and fungi has been an intense research subject; however, little is known about that of protozoa. This study investigated interaction of a representative protozoa, , with heavy elements (Eu(III), Pb(II), U(VI)). Non-destructive elemental analysis by micro-PIXE hardly detected those elements on living cells after sorption experiments but clearly detected on the cells that were killed with a fixative beforehand. Chromatographic analysis of aquatic species of those heavy elements after the sorption experiments revealed a fraction of those elements bound to a glycoprotein dissolved from the cell surface of living cells to form soluble pseudocolloid. These findings suggest that complexation of heavy elements with the dissolved surface glycoprotein reduced the sorption of those heavy elements on living cells.
Sato, Junya; Kikuchi, Hiroshi*; Kato, Jun; Sakakibara, Tetsuro; Matsushima, Ryotatsu; Sato, Fuminori; Kojima, Junji; Nakazawa, Osamu
QST-M-8; QST Takasaki Annual Report 2016, P. 62, 2018/03
no abstracts in English
Yamaguchi, Akiko*; Honda, Tasuku*; Tanaka, Masato*; Tanaka, Kazuya; Takahashi, Yoshio*
Geochemical Journal, 52(5), p.415 - 425, 2018/00
Ion-adsorption type REE deposits in weathered granite are main sources of REE essential for high-technology industries. However, these type deposits have not been searched in Japan. In this study, Bulk REE abundances (= REE), ion-exchangeable REE (= REE) by ammonium chloride solution, and percentage of REE relative to REE (= REE) in fresh and weathered granite samples in Southwest Japan (i.e., Hiroshima and Shimane Prefectures) were determined. The REE and REE were comparable to those of ion-adsorption type REE deposits in China. Extended X-ray adsorption fine structure (EXAFS) spectra of REE in original samples and samples after the extraction of ion-exchangeable REE showed that (i) REE in samples with high REE mainly forms outer-sphere complexes and (ii) the remaining REE in the rocks after the extraction forms inter-sphere complexes.
Saito, Kyoichi*; Asai, Shiho
Bunseki Kagaku, 66(11), p.771 - 782, 2017/11
Recovery and purification of rare metals, which are essential ingredients for highly functional materials, generally comes with operational difficulty. In this study, we have developed polymer adsorbents specially designed for highly-efficient adsorption of rare metal ions and exhibited their practical adsorption performances. Radiation-induced graft polymerization, one of the effective modification techniques for polymers, was employed for preparing the proposed adsorbents. Among such adsorbents, a 6-nylon fiber with nucleic-acid base, adenine, on the surface of the fiber demonstrated specific adsorption of ruthenium and palladium ions. In addition, a 6-nylon fiber with an extractant HDEHP (bis (2-ethylhexyl) phophoric acid) that has high affinity for lanthanides, achieved higher separation speed than a commercially available HDEHP-impregnated resin.
Radioisotopes, 66(11), p.601 - 610, 2017/11
no abstracts in English
Saptiama, I.*; Kaneti, Y. V.*; Suzuki, Yumi*; Suzuki, Yoshitaka; Tsuchiya, Kunihiko; Sakae, Takeji*; Takai, Kimiko*; Fukumitsu, Nobuyoshi*; Alothman, Z. A.*; Hossain, M. S. A.*; et al.
Bulletin of the Chemical Society of Japan, 90(10), p.1174 - 1179, 2017/10
no abstracts in English
Yu, Q.*; Onuki, Toshihiko*; Kozai, Naofumi; Sakamoto, Fuminori; Tanaka, Kazuya; Sasaki, Keiko*
Chemical Geology, 470, p.141 - 151, 2017/10
In this work, the Cs retention onto two types of Mn oxide was investigated. We found that Todorokite has sorption sites with a higher selectivity for Cs than birnessite. When the initial Cs concentration was 10 mol/L for the sorption experiments, approximately 34% of the sorbed Cs was residual in the todorokite after the extraction using 1 M NaCl and NHCl; this value was much higher than the results for the Cs-sorbed birnessite. These results strongly suggest that todorokite contributes to the fixation of radioactive Cs in soils.
Takahatake, Yoko; Watanabe, So; Kofuji, Hirohide; Takeuchi, Masayuki; Nomura, Kazunori; Sato, Takahiro*
International Journal of PIXE, 26(3&4), p.73 - 83, 2017/09
JAEA has been conducting research and development of MA(III) recovery from HLLW by extraction chromatography technology for reduction in amount and environmental impact of radioactive waste. The behavior of adsorbed cations inside the adsorbent packed in a column is necessary to be evaluated for improvement of the adsorbent or flow-sheet to achieve targeted MA(III) recovery performance. In this paper, micro-PIXE analysis was carried out on the particles sampled from various positions of the column to reveal the behavior of cations inside the packed column with CMPO/SiO -P adsorbent. Simple experiment and data analysis were shown to be effective to reveal inside of the column, and formation and transportation of the adsorption bands were observed for some cations which are extractable by the CMPO extractant. Some part of Zr(IV) and Mo(VI) were found to remain inside the column without distinct transportation even after the elution operation.