Molecular geochemistry developed by fluorescence XAFS using high energy resolution fluorescence X-ray detection

Yomogida, Takumi; Takahashi, Yoshio*

Chikyu Kagaku, 59(1), p.1 - 10, 2025/03

https://doi.org/10.14934/chikyukagaku.59.1

X-ray absorption fine structure XAFS spectroscopy techniques, which are applicable to almost all elements, provide information on elemental valence and local structure with high elemental selectivity and high sensitivity. It has become an indispensable method in space geochemistry and environmental chemistry. This review presents examples of the application of fluorescence XAFS methods to elements that are difficult to detect by conventional methods, and examples where new chemical species information has been obtained by increasing the energy resolution of the X-ray fluorescence (XRF) detection system to obtain XAFS.

Adsorption structures and bonding states of cesium and barium adsorbed on various sites of vermiculite

Yamaguchi, Akiko; Okumura, Masahiko; Kawamura, Naomi*; Takahashi, Yoshio*

Science of the Total Environment, 964, p.178585_1 - 178585_13, 2025/02

https://doi.org/10.1016/j.scitotenv.2025.178585

There are many unresolved issues in the adsorption reactions of clay minerals. One of the reasons is the existence of multiple adsorption sites. It is known that the contribution of each adsorption site depends on the concentration of adsorbed ions, and there is a challenge in comprehensively correlate the results of atomic-level simulations that employ limited number of atoms and inevitably deal high-concentration samples with actual environmental samples where concentrations are orders of magnitude lower. In this study, we combined experiments using synchrotron radiation and first-principles calculations to comprehensively elucidate the systematic changes in the local structure of adsorption sites and adsorbed ions based on the adsorption concentration at the atomic level, and demonstrated that the interaction between adsorbed ions and clay minerals involves ionic bonding.

Interpretation of vertical migration and enrichment processes of rare earth elements (REEs) in ion-adsorption-type mineralization in Japan based on REE speciation analyses

Nagasawa, Makoto*; Shimizu, Yusuke*; Yamaguchi, Akiko; Tokunaga, Kohei; Mukai, Hiroki*; Aoyagi, Noboru; Mei, H.; Takahashi, Yoshio*

Chemical Geology, 670, p.122431_1 - 122431_25, 2024/12

https://doi.org/10.1016/j.chemgeo.2024.122431

Circular polarization measurement for individual gamma rays in capture reactions with intense pulsed neutrons

Endo, Shunsuke; Abe, Ryota*; Fujioka, Hiroyuki*; Ino, Takashi*; Iwamoto, Osamu; Iwamoto, Nobuyuki; Kawamura, Shiori*; Kimura, Atsushi; Kitaguchi, Masaaki*; Kobayashi, Ryuju*; et al.

European Physical Journal A, 60(8), p.166_1 - 166_10, 2024/08

https://doi.org/10.1140/epja/s10050-024-01392-6

Molecular geochemistry of radium; A key to understanding cation adsorption reaction on clay minerals

Yamaguchi, Akiko; Kurihara, Yuichi*; Nagata, Kojiro*; Tanaka, Kazuya; Higaki, Shogo*; Kobayashi, Toru; Tanida, Hajime; Ohara, Yoshiyuki*; Yokoyama, Keiichi; Yaita, Tsuyoshi; et al.

Journal of Colloid and Interface Science, 661, p.317 - 332, 2024/05

https://doi.org/10.1016/j.jcis.2024.01.120

no abstracts in English

High sensitivity of a future search for effects of -odd/-odd interactions on the 0.75 eV -wave resonance in + forward transmission determined using a pulsed neutron beam

Nakabe, Rintaro*; Auton, C. J.*; Endo, Shunsuke; Fujioka, Hiroyuki*; Gudkov, V.*; Hirota, Katsuya*; Ide, Ikuo*; Ino, Takashi*; Ishikado, Motoyuki*; Kambara, Wataru*; et al.

Physical Review C, 109(4), p.L041602_1 - L041602_4, 2024/04

https://doi.org/10.1103/PhysRevC.109.L041602

The First observation of hydrated radium at the molecular level

Yamaguchi, Akiko; Okumura, Masahiko; Takahashi, Yoshio*

Isotope News, (789), p.20 - 23, 2023/10

https://www.jrias.or.jp/pdf/2310_TRACER_YAMAGUCHI_HOKA.pdf

Radium is a radioactive element produced from uranium and thorium and is important for environmental contamination issues around uranium mines and for geological disposal. In addition, radium is used in radiometric dating and cancer therapy, making it important not only in environmental chemistry but also in many other fields, including geochemistry and nuclear medicine. However, because radium is a radioactive element with no stable isotopes, spectroscopic measurement of radium is difficult, and little information at the molecular level has been obtained so far. In this study, we have clarified the molecular-level information of hydrated radium for the first time in the world by combining extended X-ray absorption fine structure (EXAFS) measurements and first-principles molecular dynamics simulations.

Improvement of the stability of IO-, SeO-, and SeO-coprecipitated barite after treatment with phosphate

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

Environmental Science & Technology, 57(8), p.3166 - 3175, 2023/02

https://doi.org/10.1021/acs.est.2c08939

Coprecipitation of radionuclides with barite has been studied to remove radionuclides from radioactive liquid waste because of its excellent removal efficiency; however, little information exists concerning the stability of the ions coprecipitated with barite. This study systematically investigated the stability of iodate, selenite, and selenate coprecipitated with barite via leaching tests. These oxyanions were gradually leached from the oxyanion-bearing barite into ultrapure water over time. Leaching of the oxyanions significantly increased in leaching solutions containing NaCl (pH5.3), NaNO (pH5.9), and NaSO (pH5.7). Conversely, leaching of the oxyanions was suppressed in KHPO solution (pH8.5), indicating that phosphate stabilized the oxyanion-bearing barite. The effect of phosphate treatment on oxyanion-bearing barite was further investigated. The results showed that the barite surface was modified with phosphate, and a thin surface layer of a barium phosphate-like structure was formed. The amount of oxyanions leached from the phosphate-treated samples into leaching solutions containing NaCl or NaNO was much lower than the amounts leached from the untreated barite samples into ultrapure water. The barite coprecipitation combined with subsequent phosphate treatment may be a promising method to efficiently remove iodate, selenite, and selenate from wastewater and stabilize them as barite coprecipitates.

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.