Yamaguchi, Akiko; Kobayashi, Keita; Takahashi, Yoshio*; Machida, Masahiko; Okumura, Masahiko
Chemical Physics Letters, 780, p.138945_1 - 138945_5, 2021/10
no abstracts in English
Konagaya, Rimi*; Kawamura, Naomi*; Yamaguchi, Akiko; Takahashi, Yoshio*
Chemistry Letters, 50(8), p.1570 - 1572, 2021/08
no abstracts in English
Tokunaga, Kohei; Takahashi, Yoshio*; Tanaka, Kazuya; Kozai, Naofumi
Chemosphere, 266, p.129104_1 - 129104_10, 2021/03
Radioactive iodine (I) is of great concern owing to its high mobility in the environment and long-term radiotoxicity, but there is a lack of effective techniques for removing iodate (IO) from aqueous solution. The aim of this study is to develop a new technique for removing radioactive iodate from contaminated solution by using barite (BaSO). In the present study, we examined the coprecipitation mechanism of iodate by barite at the molecular level for determining optimum conditions for iodate removal. The results showed that iodate was effectively removed from aqueous solution by coprecipitation, even in the presence of competitive anions in solution. Comparing our method with previous studies, iodate removal efficiency by barite was determined to be about two orders of magnitude greater than that by hydrotalcite-like layered double hydroxide at Cl concentration of 10 mmol L. Extended X-ray absorption fine structure (EXAFS) analysis indicated that incorporated iodate was strongly bound in the crystal lattice of barite by substituting the sulfate site in the structure when the iodine concentration was low. The charge compensation problem from the IO substitution in SO site is achieved by the substitution of Na-IO pairs at the nearest Ba site. Therefore, considering high removal efficiency and strong binding of iodate in barite, coprecipitation with barite is a promising material for removing radioactive iodate from various aqueous solutions contaminated with iodate.
Miyajima, Yusuke*; Saito, Ayaka*; Kagi, Hiroyuki*; Yokoyama, Tatsunori; Takahashi, Yoshio*; Hirata, Takafumi*
Geostandards and Geoanalytical Research, 45(1), p.189 - 205, 2021/03
Uncertainty for elemental and isotopic analyses of calcite by LA-ICP-MS is largely controlled by the homogeneity of the reference materials (RMs) used for normalization and validation. In order to produce calcite RMs with homogeneous elemental and isotopic compositions, we incorporated elements including U, Pb, and rare earth elements into calcite through heat- and pressure-induced crystallization from amorphous calcium carbonate that was precipitated from element-doped reagent solution. X-ray absorption spectra showed that U was present as U(VI) in the synthesized calcite, probably with a different local structure from that of aqueous uranyl ions. The uptake rate of U by our calcite was higher in comparison to synthetic calcite of previous studies. Variations of element mass fractions in the calcite were better than 12% 2RSD, mostly within 7%. The Pb/Pb ratio in the calcite showed 1% variations, while the U/Pb ratio showed 3-24% variations depending on element mass fractions. Using the synthetic calcite as primary RMs, we could date a natural calcite RM, WC-1, with analytical uncertainty as low as 3%. The method presented can be useful to produce calcite with controlled and homogeneous element mass fractions, and is a promising alternative to natural calcite RMs for U-Pb geochronology.
Miura, Hikaru*; Ishimaru, Takashi*; Ito, Yukari*; Kuribara, Yuichi; Otosaka, Shigeyoshi*; Sakaguchi, Aya*; Misumi, Kazuhiro*; Tsumune, Daisuke*; Kubo, Atsushi*; Higaki, Shogo*; et al.
Scientific Reports (Internet), 11, p.5664_1 - 5664_11, 2021/03
For the first time, we isolated and investigated seven CsMPs (radioactive caesium-bearing microparticles) from marine particulate matter and sediment. From the elemental composition, the Cs/Cs activity ratio, and the Cs activity per unit volume results, we inferred that the five CsMPs collected from particulate matter were emitted from Unit 2 of the FDNPP, whereas the two CsMPs collected from marine sediment were possibly emitted from Unit 3. The presence of CsMPs can cause overestimation of the solid-water distribution coefficient of Cs in marine sediments and particulate matter and a high apparent radiocaesium concentration factor for marine biota. CsMPs emitted from Unit 2, which were collected from the estuary of a river that flowed through a highly contaminated area, may have been deposited on land and then transported by the river. By contrast, CsMPs emitted from Unit 3 were possibly transported eastward by the wind and deposited directly onto the ocean surface.
Tanaka, Kazuya; Kanasashi, Tsutomu*; Takenaka, Chisato*; Takahashi, Yoshio*
Science of the Total Environment, 755(Part 2), p.142598_1 - 142598_8, 2021/02
In this study, we investigated coordination structures of Cs in Cs-doped bark, sapwood, heartwood, needle, and branch samples of trees collected in Fukushima by extended X-ray absorption fine structure (EXAFS) spectroscopy. We examined four representative tree species in Fukushima, , , , and . EXAFS spectra suggested that Cs was adsorbed as an outer-sphere complex on all parts of the four species, with electrostatic binding to negatively charged functional groups in components of tree tissues. These results were supported by extraction experiments where most of the sorbed Cs was desorbed from all parts of each tree species using 1 M CHCOONH.
Nagasawa, Makoto*; Qin, H.-B.*; Yamaguchi, Akiko; Takahashi, Yoshio*
Chemistry Letters, 49(8), p.909 - 911, 2020/08
Miura, Hikaru*; Kuribara, Yuichi; Yamamoto, Masayoshi*; Sakaguchi, Aya*; Yamaguchi, Noriko*; Sekizawa, Oki*; Nitta, Kiyofumi*; Higaki, Shogo*; Tsumune, Daisuke*; Itai, Takaaki*; et al.
Scientific Reports (Internet), 10, p.11421_1 - 11421_9, 2020/07
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
Igarashi, Yasuhito*; Kogure, Toshihiro*; Kuribara, Yuichi; Miura, Hikaru*; Okumura, Taiga*; Satou, Yukihiko; Takahashi, Yoshio*; Yamaguchi, Noriko*
Journal of Environmental Radioactivity, 205-206, p.101 - 118, 2019/09
Scientists face challenge in identifying the radioactive materials which are found as dotted images on various imaging plate (IP) autoradiographic photos of radioactively contaminated materials by the Fukushima Dai-ichi Nuclear Power Plant (F1NPP, or FDNPP) accident, such as air filter, fugitive dust, surface soil, agricultural materials, and water-shed samples. It has been revealed that they are minute particles with distinct morphology and elemental composition with high specific radioactivity, and different from those of the so-called Chernobyl hot particles. Basically, they are glassy particles once molten, composed of Si, O, Fe, Zn etc. with highly concentrated radiocaesium, which can be called as radiocaesium-bearing microparticles (CsMP). At present, CsMP can be classified into two types, Types-A and -B, which are characterized by different specific radioactivity, Cs/Cs ratio, size and morphology, and geographic distribution around F1NPP. Such studies on the CsMP from various aspects have provided valuable information about what happened in the nuclear reactors during the F1NPP accident and fates of the CsMP in the environment. This review first provides a retrospective view on the research history of the CsMP, which is helpful to understand the unique character of the CsMP. Subsequently, more details about the current understanding of the natures of these hot particles, such as origin, morphology, chemical compositions, thermal properties, water-solubility, and secondary migration of CsMP in river and ocean systems are described with future prospects.
Tanaka, Kazuya; Takahashi, Yoshio*
Geochemical Journal, 53(5), p.329 - 331, 2019/00
We examined three natural zircon samples with different amounts of radiation doses using M-edge and L-edge U X-ray absorption near-edge structure (XANES). Analysis of XANES spectra at both M-edge and L-edge suggested that the oxidation state of U in the zircon sample with the highest radiation dose is tetravalent. The XANES spectra of the two other samples with lower radiation doses suggested a mixture of U(IV) and U(VI), while the possibility of U(V) was not excluded. This is the first work on the application of M-edge U XANES to the oxidation state of U in natural zircon.
Tokunaga, Kohei; Kozai, Naofumi; Takahashi, Yoshio*
Journal of Hazardous Materials, 359, p.307 - 315, 2018/07
In the present study, we looked at the removal efficiency of Sr by using barite (BaSO) under various experimental conditions to develop techniques for the direct removal of Sr from seawater. The uptake of Sr by barite was found to be dependent on pH, saturation state, and [Ba]/[SO] ratio in initial aqueous solution, showing that most of the aqueous Sr can be removed from the aqueous solution by adjusting these parameters. However, the effects of ionic strength and competitive ions were negligible, suggesting the effectiveness of its application to removal of Sr from seawater. Batch experiments were also conducted in a seawater system, and a rather high removal efficiency of Sr from seawater (more than 90%) was achieved. Considering its high removal and retention efficiency of Sr in seawater systems, barite is a reliable material for the removal of Sr from seawater.
Tanaka, Kazuya; Watanabe, Naoko*; Yamasaki, Shinya*; Sakaguchi, Aya*; Fan, Q.*; Takahashi, Yoshio*
Geochemical Journal, 52(2), p.173 - 185, 2018/00
We analyzed riverbed sediments collected at two sites, Yamakiya and Kuroiwa, in Fukushima after the Fukushima accident. The size distributions of K, Rb, and Csreflected the mineralogy of sediments, where primary host minerals for these alkali elements would be biotite, K-feldspar, and clay minerals. Silt-size fractions contained high Cs and Cs concentrations possibly due to adsorption on clay minerals. Their concentrations decreased with particle size at the Yamakiya site. In contrast, coarse and very coarse sand fractions from the Kuroiwa site showed higher Cs and Cs concentrations in comparison to fine - medium sand fractions. The coarse sand fractions contained many weathered biotite grains. Overall, the size distributions of Cs and Cs were similar in the sediments, suggesting that the Fukushima-derived radiocesium was distributed into each particle size fraction in response to the distribution of the stable Cs that was controlled by mineralogical composition.
Sakaguchi, Aya*; Chiga, Haruka*; Tanaka, Kazuya; Tsuruta, Haruo*; Takahashi, Yoshio*
Geochemical Journal, 52(2), p.187 - 199, 2018/00
An aerosol sample collected on the 15th of March 2011 at Kawasaki City (Kanagawa) was sequentially leached with seawater for 30 days. As a result, about 60% of the total Cs was extracted. In addition, a surface soil sample collected from Kawamata Town (Fukushima) two months after the Fukushima accident, was leached for 223 days with a natural seawater, a 1:1 mixture of ultrapure water and seawater, and ultrapure water. Eventually, more than 15% of the total Cs in the surface soil sample was efficiently desorbed by seawater leaching. In comparison, about 9% of the total Cs was leached with 1:1 diluted seawater and less than 1% of the total Cs was leached with ultrapure water over the 223 days. Overall, Cs and Cs showed similar leaching behaviour.
Miura, Hikaru*; Kurihara, Yuichi*; Sakaguchi, Aya*; Tanaka, Kazuya; Yamaguchi, Noriko*; Higaki, Shogo*; Takahashi, Yoshio*
Geochemical Journal, 52(2), p.145 - 154, 2018/00
Solid-water distribution coefficient () of radiocesium in rivers is apparently increased due to the possible presence of highly radioactive radiocesium-bearing microparticles (CsMPs) in the solid phase. In this study, we evaluated the contribution of CsMPs to apparent Kd values. The ratio of the radioactivity of the separated CsMPs to the total radiocesium on fluvial suspended particles ranged from 0 to 46%. This means that the existence of CsMPs in fluvial suspended partcles did not change apparent Kd values in order magnitude.
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.
Takahashi, Yoshio*; Fan, Q.*; Suga, Hiroki*; Tanaka, Kazuya; Sakaguchi, Aya*; Takeichi, Yasuo*; Ono, Kanta*; Mase, Kazuhiko*; Kato, Kenji*; Kanivets, V. V.*
Scientific Reports (Internet), 7(1), p.12407_1 - 12407_11, 2017/09
We focused on factors controlling partition of radiocesium on particulate matters and sediments in rivers of Fukushima and Chernobyl. Radiocesium is more soluble in the Pripyat River (Chernobyl) due to weaker interaction of radiocesium with clay minerals caused by the inhibition effect of the adsorbed humic substances. In contrast, particulate matters and sediments in the Kuchibuto River (Fukushima) display high adsorption affinity with lesser inhibition effect of adsorbed humic substances. This difference is possibly governed by the geology and soil type of provenances surrounding both catchments.
Tokunaga, Kohei*; Takahashi, Yoshio*
Environmental Science & Technology, 51(16), p.9194 - 9201, 2017/08
In the present study, we explore a new application of barite (BaSO) as a sequestering phase for selenite (Se(IV)) and selenate (Se(VI)) ions from aqueous solutions due to the low solubility and high stability of barite. The uptake of Se(IV) and Se(VI) during coprecipitation with barite was investigated through batch experiments to understand the factors controlling effective removal of Se(IV) and Se(VI) from polluted water to barite. The uptake of Se(IV) by barite is dependent on pH, coexistent calcium ion, and sulfate concentration in the initial solution, possibly due to their effects on the chemical affinity and structural similarity. On the other hand, the uptake of Se(VI) by barite was strongly dependent on sulfate concentration in the initial solution, which is only related to the structural similarity. This study provides a good estimate of its ability to effectively remove Se(IV) and Se(VI) from aqueous solutions (more than 80%) under optimized experimental parameters.
Tanaka, Kazuya; Tanaka, Masato*; Watanabe, Naoko*; Tokunaga, Kohei*; Takahashi, Yoshio*
Chemical Geology, 460, p.130 - 137, 2017/06
Pd is highly accumulated in ferromanganese nodules and crusts relative to its concentration in seawater but the mechanism by which Pd(II) is incorporated remains poorly understood. We investigated the local coordination structure of Pd(II) adsorbed on -MnO, using X-ray absorption fine structure spectroscopy. X-ray absorption near edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) analyses indicated that Pd was adsorbed on -MnO through ligand exchange, from Cl coordination to O coordination. Furthermore, curve fitting of EXAFS spectra demonstrated the formation of two different inner-sphere complexes, bidentate-mononuclear and bidentate-binuclear complexes, and this finding was supported by density functional theory calculations. The formation of inner-sphere complexes is reasonable given the relatively large distribution coefficients obtained from adsorption experiments.
Fujimoto, Jun*; Tanaka, Kazuya; Watanabe, Naoko*; Takahashi, Yoshio*
Hydrometallurgy, 166, p.80 - 86, 2016/12
We examined recovery of REEs in Fe-Mn nodules by using (Fe-reducing bacterium). In this method, Fe-Mn nodule decomposition and REE recovery were achieved simultaneously in a single solution system. Fe-Mn nodules were reductively decomposed in NaCl solution under anaerobic conditions with daily addition of sodium lactate as an electron donor. During the decomposition of Fe-Mn nodule, REEs released from the Fe-Mn nodule were adsorbed on bacterial cells. Of the conditions studied here, the best REE adsorption rates were obtained with 0.5M NaCl solution at pH7 with daily addition of 1 mmol sodium lactate.