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Kato, Tomoaki; Kozai, Naofumi; Tanaka, Kazuya; Kaplan, D. I.*; Utsunomiya, Satoshi*; Onuki, Toshihiko
Journal of Nuclear Science and Technology, 59(5), p.580 - 589, 2022/05
This study reports the effect of fulvic acids, which is a natural organic substance generally contained in groundwater, on the oxidation states of radioactive iodine anions (iodide and iodate). Iodide and iodate are contained in the contaminated water of the Fukushima Daiichi Nuclear Power Plant and supposed to be removed by activated carbon (AC) via adsorption. When fulvic acids does not exist in the experimental system, the adsorption of iodide on AC was less than that of iodate and their oxidation states after the adsorption were not changed. When fulvic acids existed, a fraction of the adsorbed iodate was reduced to iodide. This result indicates that the reduction of the adsorbed iodate progresses during the storage of the spent AC.
C control rods in Fukushima Daiichi nuclear reactors during meltdown; B-Li isotopic signatures in cesium-rich microparticlesFueda, Kazuki*; Takami, Ryu*; Minomo, Kenta*; Morooka, Kazuya*; Horie, Kenji*; Takehara, Mami*; Yamasaki, Shinya*; Saito, Takumi*; Shiotsu, Hiroyuki; Onuki, Toshihiko*; et al.
Journal of Hazardous Materials, 428, p.128214_1 - 128214_10, 2022/04
Tanaka, Kazuya; Tani, Yukinori*; Kozai, Naofumi; Onuki, Toshihiko
Journal of Radioanalytical and Nuclear Chemistry, 331(2), p.1109 - 1114, 2022/02
We investigated the sorption of Pu(IV) on biogenic Mn oxide produced by Mn(II)-oxidizing fungus. The sorption of Pu(IV) on biogenic Mn oxide was similar to that of U(VI) and different from that of Th(IV), possibly due to oxidation of Pu(IV) to Pu(VI). When Pu(IV) was sorbed on hyphae only, it was desorbed into the solution phase over time. Pu(IV) could be solubilized by complexation with organic ligands secreted by fungal cells. In particular, Pu(IV) desorption was observed under circumneutral pH conditions.
Grambow, B.; Nitta, Ayako; Shibata, Atsuhiro; Koma, Yoshikazu; Utsunomiya, Satoshi*; Takami, Ryu*; Fueda, Kazuki*; Onuki, Toshihiko*; Jegou, C.*; Laffolley, H.*; et al.
Journal of Nuclear Science and Technology, 59(1), p.1 - 24, 2022/01
Times Cited Count：0 Percentile：0.37(Nuclear Science & Technology)Kozai, Naofumi; Sato, Junya; Osugi, Takeshi; Shimoyama, Iwao; Sekine, Yurina; Sakamoto, Fuminori; Onuki, Toshihiko
Journal of Hazardous Materials, 416, p.125965_1 - 125965_9, 2021/08
Times Cited Count：1 Percentile：0(Engineering, Environmental)Deng, G.*; Ma, T.*; Tanaka, Kazuya; Onuki, Toshihiko*; Qiu, X.*; Yu, Q.*
Geochimica et Cosmochimica Acta, 286, p.143 - 158, 2020/10
Times Cited Count：0 Percentile：0.01(Geochemistry & Geophysics)In this study, Ce(III) adsorption on Mn(IV) oxide was investigated in the presence of dextran, one of polysaccharides. As a result, Ce(IV) on Mn(IV) oxide was solubilized by the complexation with dextran.
Guo, B.*; Xiong, Y.*; Chen, W.*; Saslow, S. A.*; Kozai, Naofumi; Onuki, Toshihiko*; Dabo, I.*; Sasaki, Keiko*
Journal of Hazardous Materials, 389, p.121880_1 - 121880_11, 2020/05
Times Cited Count：20 Percentile：95.57(Engineering, Environmental)
on Ni-Zn layered hydroxide salt and its application to removal of ReO as a surrogate of TcOTanaka, Kazuya; Kozai, Naofumi; Yamasaki, Shinya*; Onuki, Toshihiko; Kaplan, D. I.*; Grambow, B.
Applied Clay Science, 182, p.105282_1 - 105282_8, 2019/12
Times Cited Count：5 Percentile：57.36(Chemistry, Physical)In this study, Ni-Zn layered hydroxide salt (LHS) was used for adsorption experiments of ReO, as a surrogate of TcO, in aqueous solutions with various initial Re and sodium salt concentrations. The maximum adsorption amount of Re was estimated at 127.7 mg/g (6.86 
10
eq/g) by fitting adsorption isotherm of ReO to Langmuir plot. The adsorption of ReO at neutral pH was a reversible process by anion exchange, and decreased with increasing Cl, NO
and SO
in solution. EXAFS analysis indicated that ReO was adsorbed as an outer-sphere complex on Ni-Zn LHS. The Ni-Zn LHS is a more robust adsorbent for ReO than the Mg-Al LDH in terms of solution pH and tolerance to competing anions, and may be an effective alternative to the traditional and more limited method of removing aqueous TcO by reductive precipitation.
, Zn
+, and CoKato, Tomoaki*; Yu, Q.*; Tanaka, Kazuya; Kozai, Naofumi; Saito, Takumi*; Onuki, Toshihiko
Journal of Environmental Sciences, 86, p.78 - 86, 2019/12
Times Cited Count：0 Percentile：0(Environmental Sciences)This paper investigated the fate of the dissolved permanganate in aqueous solution after contact with bacterial cells and metal accumulation during precipitation of Mn oxides. When Mn(VII) was contacted with bacterial cells, cells were damaged and Mn(VII) was reduced by cells to lower valence and precipitated as Mn oxides (biomass Mn oxides). When Co ions were present, Co was incorporated into Mn oxides as Co
. These results suggest that Mn(VII) can be used to remove metal ions when introduced to wastewater as disinfectant.
Onuki, Toshihiko*; Satou, Yukihiko; Utsunomiya, Satoshi*
Journal of Nuclear Science and Technology, 56(9-10), p.790 - 800, 2019/09
Times Cited Count：1 Percentile：26.54(Nuclear Science & Technology)
investigation of radioactive Cs mobility around litter zone in contaminated forest using spent mushroom substrataOnuki, Toshihiko*; Sakamoto, Fuminori; Kozai, Naofumi; Yamasaki, Shinya*; Sasaki, Yoshito; Niizato, Tadafumi
Journal of Nuclear Science and Technology, 56(9-10), p.814 - 821, 2019/09
Times Cited Count：0 Percentile：0.01(Nuclear Science & Technology)We used the spent mushroom substrata (SMSs) which are a kind of by-product after growing edible mushrooms for the 
investigation of radioactive Cs mobility in litter zone in a forest of Fukushima prefecture, Japan. The powder SMS was filled in a plastic net bag of 0.350.55 m, then was placed in a forest for 
6 months under three kinds of different conditions without treatment (No treatment), covered with wooden box (With box), and with zeolite placed on upper position of ground surface (With zeolite). We determined the ratio of radioactivity (TF) in the SMS to that of the soil and litter beneath the SMS bags. TFs of "No treatment" and of "With zeolite" were determined between 0.01 and 0.05 for 6 months. On the other hand, TFs of "With box" were lower by one order at 2 and 4 months than those of "No treatment" and of "With zeolite", and nearly the same values as TFs of "No treatment" and "With zeolite" at 6 months. These results clearly indicate that radioactive Cs accumulates in SMS mainly by throughfall. In addition, for a period of several months, fungi contribute to the accumulation of radioactive Cs in the litter zone, even though radioactive Cs was tightly associated with the soil.
Onuki, Toshihiko; Sakamoto, Fuminori; Kozai, Naofumi; Namba, Kenji*; Neda, Hitoshi*; Sasaki, Yoshito; Niizato, Tadafumi; Watanabe, Naoko*; Kozaki, Tamotsu*
Environmental Science; Processes & Impacts, 21(7), p.1164 - 1173, 2019/07
Times Cited Count：7 Percentile：53.88(Chemistry, Analytical)The fate of radioactive Cs deposited after the Fukushima nuclear power plant accident and its associated radiological impacts are largely dependent on its mobility from surface soils to forest ecosystems. We measured the accumulation of radioactive Cs in the fruit bodies of wild fungi in the forest at Iidate, Fukushima, Japan. The transfer factors (TFs) of radioactive Cs from soil to the fruit bodies of wild fungi were between 10 
to 10, a range similar to those reported for the fruit bodies collected in Europe after the Chernobyl accident and in parts of Japan contaminated by nuclear bomb test fallout. Comparison of the TFs of the wild mushroom and that of the fungal hyphae of 704 stock strains grown on agar medium containing nutrients and radioactive Cs showed that the TFs of wild mushroom were lower. TF was less than 0.1 after addition of the minerals zeolite, vermiculite, phlogopite, smectite, or illite of 1% weight to the agar medium. These results indicate that the presence of minerals decrease Cs uptake by fungi grown in the agar medium.
Liu, J.; Dotsuta, Yuma; Kitagaki, Toru; Kozai, Naofumi; Yamaji, Keiko*; Onuki, Toshihiko
Proceedings of International Topical Workshop on Fukushima Decommissioning Research (FDR 2019) (Internet), 2 Pages, 2019/05
To decommission the Fukushima Daiichi Nuclear Power Plant (FDNPP), it is necessary to estimate the current status of fuel debris and predicate the possible change under various condition. Some microorganisms may enter the plant due to the seawater injection after accident and future defueling activity. In this study, microbial influence on fuel debris under aerobic condition was experimentally investigated. By culturing some bacteria in the presence of simulant fuel debris in liquid medium, the microbial degradation of fuel debris was observed.
Tanaka, Kazuya; Kozai, Naofumi; Onuki, Toshihiko; Grambow, B.
Journal of Porous Materials, 26(2), p.505 - 511, 2019/04
Times Cited Count：6 Percentile：50.98(Chemistry, Applied)In this study, we utilized X-ray absorption fine structure spectroscopy to clarify the coordination structure of Re in Mg-Al LDH as a surrogate of Tc. Adsorption experiments of ReO on calcined and uncalcined Mg-Al LDHs were conducted in aqueous solutions with different concentrations of NaCl, NaNO, and Na
SO. Calcined Mg-Al LDH showed much higher adsorption than uncalcined one. The adsorption of ReO was reversible, and decreased with increasing concentration of competing anions like Cl, NO, or SO. Analysis of Re L
-edge extended X-ray absorption fine structure indicated that ReO was adsorbed as an outer-sphere complex on Mg-Al LDH. The observed Re adsorption-desorption behavior, which was sensitive to the presence of competing anions, was consistent with the formation of outer sphere-complex.
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.
glycoprotein; Microbial transformation of heavy elements in the aquatic environmentKozai, Naofumi; Sakamoto, Fuminori; Tanaka, Kazuya; Onuki, Toshihiko; Sato, Takahiro*; Kamiya, Tomihiro*; Grambow, B.
Chemosphere, 196, p.135 - 144, 2018/04
Times Cited Count：2 Percentile：13.2(Environmental Sciences)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.
Tanaka, Kazuya; Kaplan, D. I.*; Onuki, Toshihiko
Applied Geochemistry, 85(Part B), p.119 - 120, 2017/10
Times Cited Count：0 Percentile：0.3(Geochemistry & Geophysics)We have prepared a special issue for Applied Geochemistry entitled "Transformation and Fate of Natural and Anthropogenic Radionuclides in the Environments". Here, we present 13 peer-reviewed articles on the general theme of natural and anthropogenic radionuclides in different environments. At the same time, these articles cover various topics of field research on the distribution of radionuclides, as well as laboratory experiments on adsorption and redox chemistry of these. The articles have been written by the attendees of the session at the Goldschmidt 2016 held in Yokohama, Japan, and by other authors who submitted their manuscripts to Applied Geochemistry focusing on the theme of the special issue.
Horiike, Takumi*; Dotsuta, Yuma*; Nakano, Yuriko*; Ochiai, Asumi*; Utsunomiya, Satoshi*; Onuki, Toshihiko; Yamashita, Mitsuo*
Applied and Environmental Microbiology, 83(20), p.e00855-17_1 - e00855-17_11, 2017/10
Times Cited Count：8 Percentile：50.78(Biotechnology & Applied Microbiology)Radioactive strontium (
Sr) leaked into the ocean from the Fukushima Daiichi Nuclear Power Plant after the nuclear accident. Since the removal of Sr using general adsorbents is not efficient at high salinity, this study investigated removal of soluble Sr from a saline solution by biogenic carbonate minerals. An isolate, Bacillus sp. strain TK2d, from marine sediment removed more than 99 % of Sr in a saline solution. Sr adsorbed at the cell surface and then carbonate minerals containing Sr developed outside the cells.
Yu, Q.*; Onuki, Toshihiko*; Kozai, Naofumi; Sakamoto, Fuminori; Tanaka, Kazuya; Sasaki, Keiko*
Chemical Geology, 470, p.141 - 151, 2017/10
Times Cited Count：7 Percentile：39.47(Geochemistry & Geophysics)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.
Onuki, Toshihiko; Kozai, Naofumi; Sakamoto, Fuminori; Utsunomiya, Satoshi*; Kato, Kenji*
Chemistry Letters, 46(5), p.771 - 774, 2017/05
Times Cited Count：0 Percentile：0(Chemistry, Multidisciplinary)The sorption behavior of Np(V) by the microbe consortia and by a single pure culture of Fe reducing bacterium was studied at pH between 3 and 7 in resting cell conditions. The sorption of Np(V) by the Fe reducing bacterium obtained in the inert condition and by the consortia in aerated condition were higher than by the Fe reducing bacterium in aerobic condition at pH below 5, strongly suggesting presence of other mechanism than the adsorption on microbial cell surface, i.e. reduction to Np(IV).
