Application of high-energy-resolution X-ray absorption spectroscopy at the U L-edge to assess the U(V) electronic structure in FeUO

Yomogida, Takumi; Akiyama, Daisuke*; Ouchi, Kazuki; Kumagai, Yuta; Higashi, Kotaro*; Kitatsuji, Yoshihiro; Kirishima, Akira*; Kawamura, Naomi*; Takahashi, Yoshio*

Inorganic Chemistry, 61(50), p.20206 - 20210, 2022/12

https://doi.org/10.1021/acs.inorgchem.2c03208

FeUO was studied to clarify the electronic structure of U(V) in a metal monouranate compound. We obtained the peak splitting of HERFD-XANES spectra utilizing high-energy-resolution fluorescence detection-X-ray absorption near edge structure (HERFD-XANES) spectroscopy at the U L-edge, which is a novel technique in the U(V) compounds. Theoretical calculations revealed that the peak splitting was caused by splitting the 6d orbital of U(V). Such distinctive electronic states are of major interest to researchers and engineers working in various fields, from fundamental physics to the nuclear industry and environmental sciences for actinide elements.

Design and actual performance of J-PARC 3 GeV rapid cycling synchrotron for high-intensity operation

Yamamoto, Kazami; Kinsho, Michikazu; Hayashi, Naoki; Saha, P. K.; Tamura, Fumihiko; Yamamoto, Masanobu; Tani, Norio; Takayanagi, Tomohiro; Kamiya, Junichiro; Shobuda, Yoshihiro; et al.

Journal of Nuclear Science and Technology, 59(9), p.1174 - 1205, 2022/09

https://doi.org/10.1080/00223131.2022.2038301

In the Japan Proton Accelerator Research Complex, the purpose of the 3 GeV rapid cycling synchrotron (RCS) is to accelerate a 1 MW, high-intensity proton beam. To achieve beam operation at a repetition rate of 25 Hz at high intensities, the RCS was elaborately designed. After starting the RCS operation, we carefully verified the validity of its design and made certain improvements to establish a reliable operation at higher power as possible. Consequently, we demonstrated beam operation at a high power, namely, 1 MW. We then summarized the design, actual performance, and improvements of the RCS to achieve a 1 MW beam.

Microbial influences on manganese deposit formation at Yunotaki Fall, Japan

Shiraishi, Fumito*; Chihara, Ryoji*; Tanimoto, Risa*; Tanaka, Kazuya; Takahashi, Yoshio*

Island Arc, 31(1), p.e12448_1 - e12448_9, 2022/05

https://doi.org/10.1111/iar.12448

At Yunotaki Fall in north Japan, manganese-oxidizing bacteria were previously assumed to have oxidized manganese to precipitate birnessite, which relied on oxygen released from algae. However, it remained unclear whether larger-scale manganese oxide precipitation was actually occurring under light conditions. This study evaluated the contribution of indirect oxidation using microelectrodes to analyze local water chemistry, in addition to bulk water chemistry and DNA analyses. The results of this study demonstrate that low bulk pH values in the hot spring water hindered indirect oxidation despite the occurrence of active oxygenic photosynthesis and that direct oxidation by manganese-oxidizing bacteria is considered to dominate in the investigated sample.

Investigation of hydration and adsorption structures on clay minerals of radium by EXAFS

Yamaguchi, Akiko; Nagata, Kojiro*; Tanaka, Kazuya; Kobayashi, Keita; Kobayashi, Toru; Shimojo, Kojiro; Tanida, Hajime; Sekiguchi, Tetsuhiro; Kaneta, Yui; Matsuda, Shohei; et al.

Hosha Kagaku, (45), p.28 - 30, 2022/03

no abstracts in English

Hydration structures of barium ions; molecular dynamics simulations using the SCAN meta-GGA density functional and EXAFS spectroscopy studies

Yamaguchi, Akiko; Kobayashi, Keita; Takahashi, Yoshio*; Machida, Masahiko; Okumura, Masahiko

Chemical Physics Letters, 780, p.138945_1 - 138945_5, 2021/10

https://doi.org/10.1016/j.cplett.2021.138945

no abstracts in English

Effective removal of iodate by coprecipitation with barite; Behavior and mechanism

Tokunaga, Kohei; Takahashi, Yoshio*; Tanaka, Kazuya; Kozai, Naofumi

Chemosphere, 266, p.129104_1 - 129104_10, 2021/03

https://doi.org/10.1016/j.chemosphere.2020.129104

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.

Thermally altered subsurface material of asteroid (162173) Ryugu

Kitazato, Kohei*; Milliken, R. E.*; Iwata, Takahiro*; Abe, Masanao*; Otake, Makiko*; Matsuura, Shuji*; Takagi, Yasuhiko*; Nakamura, Tomoki*; Hiroi, Takahiro*; Matsuoka, Moe*; et al.

Nature Astronomy (Internet), 5(3), p.246 - 250, 2021/03

https://doi.org/10.1038/s41550-020-01271-2

Here we report observations of Ryugu's subsurface material by the Near-Infrared Spectrometer (NIRS3) on the Hayabusa2 spacecraft. Reflectance spectra of excavated material exhibit a hydroxyl (OH) absorption feature that is slightly stronger and peak-shifted compared with that observed for the surface, indicating that space weathering and/or radiative heating have caused subtle spectral changes in the uppermost surface. However, the strength and shape of the OH feature still suggests that the subsurface material experienced heating above 300 C, similar to the surface. In contrast, thermophysical modeling indicates that radiative heating does not increase the temperature above 200 C at the estimated excavation depth of 1 m, even if the semimajor axis is reduced to 0.344 au. This supports the hypothesis that primary thermal alteration occurred due to radiogenic and/or impact heating on Ryugu's parent body.

Speciation of cesium in tree tissues and its implication for uptake and translocation of radiocesium in tree bodies

Tanaka, Kazuya; Kanasashi, Tsutomu*; Takenaka, Chisato*; Takahashi, Yoshio*

Science of the Total Environment, 755(Part 2), p.142598_1 - 142598_8, 2021/02

https://doi.org/10.1016/j.scitotenv.2020.142598

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.

Characterization of two types of cesium-bearing microparticles emitted from the Fukushima accident via multiple synchrotron radiation analyses

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

https://doi.org/10.1038/s41598-020-68318-2

A Review of Cs-bearing microparticles in the environment emitted by the Fukushima Dai-ichi Nuclear Power Plant accident

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

https://doi.org/10.1016/j.jenvrad.2019.04.011

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.