Design of the SPring-8 JAEA beamline BL22XU

Shiwaku, Hideaki; Marushita, Motoharu*

JAEA-Research 2022-015, 39 Pages, 2023/05

JAEA-Research-2022-015.pdf:2.74MB

We designed the hard X-ray undulator beamline BL22XU, which is dedicated to Japan Atomic Energy Research Institute (JAERI) at SPring-8 (now Japan Atomic Energy Agency (JAEA)). BL22XU is used for XAFS (X-ray Absorption Fine Structure) analysis experiments to develop separation and extraction materials for radioactive waste treatment and to elucidate their chemical behavior, magnetic research experiments using a diffractometer, and experiments under extreme conditions using a high-pressure press and a diamond anvil cell. The available X-ray energy range was set from 3 to 70 keV. To design the optics of the beamline, the reflectivity of the mirrors, the diffraction width of the monochromatic crystal, and the absorptance of the Be window were calculated. In addition, ray tracing was performed to optimize the materials for optics, dimensions, and location. The delay time of the ADL (Acoustic Delay Line) was also examined to ensure the safety in the use of radioactive materials. The operation of BL22XU "JAEA Actinide Science I" has already started. By collaborating BL22XU and BL23SU "JAEA Actinide Science II," which uses a soft X-ray undulator as a light source, we solve the problems to promote nuclear sciences. Since the monochromator was upgraded in 2018-2019, initial planning and measured data are documented here again.

Structural change by phosphorus addition to borosilicate glass containing simulated waste components

Okamoto, Yoshihiro; Shiwaku, Hideaki; Shimamura, Keisuke*; Kobayashi, Hidekazu; Nagai, Takayuki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*

Journal of Nuclear Materials, 570, p.153962_1 - 153962_13, 2022/11

https://doi.org/10.1016/j.jnucmat.2022.153962

Simulated nuclear waste glass samples containing phosphorus, which increase the solubility of molybdenum, were prepared and analyzed using synchrotron X-ray Absorption Fine Structure (XAFS) analysis for some constituent elements and Raman spectroscopic analysis of their complex structure. Changes in local structure and chemical state due to different phosphorus additions and waste loading rates were systematically studied. Consequently, no crystalline phase due to the molybdate compound was observed even at a maximum waste content of 30 wt% (corresponding to 1.87 mol% MoO). Oxidation proceeded when the waste-loading rate was increased, whereas the reduction proceeded when phosphorus was added. In some cases, the effects of oxidation and reduction were offset. The local structure around specific elements can be classified as follows; Zn that is affected mainly by the waste-loading rate, Ce that is affected by both the waste-loading rate and phosphorus addition, and Zr element that is not affected by either of them. From the comparison between the analytical results of Mo and other elements, it was considered that the added phosphorus exists as a free PO structural unit and may deprive the alkali metal coordinated to the molybdate ion.

Transfer behavior of cesium adsorbed on clay minerals in aqueous solution

Okamoto, Yoshihiro; Osugi, Takeshi; Shiwaku, Hideaki; Akabori, Mitsuo*

Insights Concerning the Fukushima Daiichi Nuclear Accident, Vol.4; Endeavors by Scientists, p.285 - 294, 2021/10

The transfer behavior of cesium adsorbed on some clay minerals in aqueous solution was investigated by X-ray absorption fine structure (XAFS) analysis of the Cs K-edge. The sample was prepared by mixing Cs-adsorbed mineral with a different pure clay mineral in water. The XAFS results of the dried mixture powder were compared with those obtained before mixing. It was recognized from the XAFS analysis for three kinds of clay minerals illite, kaolinite and vermiculite, that cesium was transferred from kaolinite to illite and vermiculite, and from illite to vermiculite. It can be concluded that cesium is transferred to and accumulated in vermiculite.

XAFS analysis of ruthenium in simulated iron phosphate radioactive waste glass

Okamoto, Yoshihiro; Kobayashi, Hidekazu; Shiwaku, Hideaki; Sasage, Kenichi; Hatakeyama, Kiyoshi*; Nagai, Takayuki

Journal of Non-Crystalline Solids, 551, p.120393_1 - 120393_8, 2021/01

https://doi.org/10.1016/j.jnoncrysol.2020.120393

The chemical state of ruthenium in simulated iron phosphate radioactive waste glass was investigated by conventional X-ray absorption fine structure (XAFS) and imaging XAFS analyses. The EXAFS analysis suggested that ruthenium was contained as glass phase when content of the waste components was less than 10wt.% in 30 mol%FeO-PO base glass. In other samples, crystalline RuO was predominant. According to the imaging XAFS analysis, RuO particles in all samples had length smaller than 50m. Aggregations of RuO, which are found in nuclear waste borosilicate glass, were not seen in any of the iron phosphate glass samples.

Interaction of Fe and Si under anoxic and reducing conditions; Structural characteristics of ferrous silicate co-precipitates

Francisco, P. C. M.; Mitsui, Seiichiro; Ishidera, Takamitsu; Tachi, Yukio; Doi, Reisuke; Shiwaku, Hideaki

Geochimica et Cosmochimica Acta, 270, p.1 - 20, 2020/02

https://doi.org/10.1016/j.gca.2019.11.009

Synchrotron radiation-based techniques available at JAEA advanced characterization nanotechnology platform (Japan Atomic Energy Agency)

Yoneda, Yasuhiro; Yoshigoe, Akitaka; Takeda, Yukiharu; Shiwaku, Hideaki; Matsumura, Daiju; Shobu, Takahisa; Tamura, Kazuhisa

Materia, 58(12), p.763 - 769, 2019/12

https://doi.org/10.2320/materia.58.763

This is an introduction to the equipment provided for each implementation period belonging to the structure analysis platform in the nanotechnology platform.

Proton chelating ligands drive improved chemical separations for rhodium

Narita, Hirokazu*; Nicolson, R. M.*; Motokawa, Ryuhei; Ito, Fumiyuki*; Morisaku, Kazuko*; Goto, Midori*; Tanaka, Mikiya*; Heller, W. T.*; Shiwaku, Hideaki; Yaita, Tsuyoshi; et al.

Inorganic Chemistry, 58(13), p.8720 - 8734, 2019/07

https://doi.org/10.1021/acs.inorgchem.9b01136

Synchrotron radiation based XAFS analysis of the simulated nuclear waste glass samples prepared by bottom drain test in the full-scale mock-up melter (KMOC) (Contract research)

Okamoto, Yoshihiro; Nagai, Takayuki; Shiwaku, Hideaki; Kano, Shigeru; Himeno, Haruyuki*; Kobayashi, Hiroshi*; Nakatani, Mikio*

JAEA-Research 2018-013, 18 Pages, 2019/03

JAEA-Research-2018-013.pdf:1.98MB

The chemical state and local structure of some elements in the simulated nuclear waste glass samples (20 batches) prepared by bottom drain test in the full scale mock-up tests using KMOC melter were investigated by synchrotron radiation based X-ray absorption fine structure (XAFS) analysis. As a result of the analysis of cerium element, it was confirmed that the oxidation proceeds gently as the batch advanced. For manganese, iron, and zinc, there was almost no difference between batches, which seemed to be stabilized by getting into the frame structure of the borosilicate glass. There were no elements that seemed to be clearly crystalline except for platinum group elements. Remarkable precipitation was hardly observed in zirconium and molybdenum with the imaging analysis.

Complexation properties and structural character of lanthanides complexes of -hetero donor ligand BIZA

Kobayashi, Toru; Akutsu, Kazuhiro*; Nakase, Masahiko*; Suzuki, Shinichi; Shiwaku, Hideaki; Yaita, Tsuyoshi

Separation Science and Technology, 54(13), p.2077 - 2083, 2019/02

https://doi.org/10.1080/01496395.2019.1575880

Development of separation reagent, which can efficiently separate lanthanides, is of increasing importance because it concerns establishment of purification and recycle techniques rare-earth elements. In our research group, several hetero donor type ligands, which have both oxygen and heterocyclic nitrogen atoms as donor atoms, were developed and revealed that this type of ligands show the selective complexation with specific lanthanide. In this paper, we will discuss the lanthaides complexation properties of the hetero donor type ligand containing benzimidazole group as nitrogen donor (-methyl--phenyl-2-(1-benzimidazol-2-yl)-pyridine-6-carboxamide) based on structural investigation by crystallography.

Investigation of simulated waste glass samples prepared from borosilicate glass frit including vanadium

Nagai, Takayuki; Okamoto, Yoshihiro; Shiwaku, Hideaki; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*; Hirono, Kazuya*; Homma, Masanobu*; Kobayashi, Hiromi*; Takahashi, Tomoe*; et al.

JAEA-Research 2018-007, 87 Pages, 2018/11

JAEA-Research-2018-007.pdf:61.21MB

To select the chemical composition of a glass frit which can increase the waste content, the simulated waste glass samples prepared from a borosilicate glass frit including vanadium (V) were investigated by using Laser Ablation (LA) ICP-AES analysis, Raman spectrometry, and synchrotron XAFS measurement in this study on foundation business of the Agency for Natural Resources and Energy.