Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 4 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

JAEA-Research 2024-014, 54 Pages, 2025/02

JAEA-Research-2024-014.pdf:7.02MB

XAFS measurements in the soft X-ray region are suitable for evaluating the chemical state of the surface layer of a measurement sample because the X-ray transmittance is low. In this study, the purpose of the study was to confirm the difference between the coagulated surface layer and the inside of the simulated waste glasses by measuring the K-edge of the glass constituent elements boron, oxygen, sodium, and silicon, and the L edge of the waste component cerium. As a result, the B K-edge XANES spectra showed that the proportion of B-O tetracoordinate sp structures (BO) on the surface layer of the coagulated glass samples was higher than that on the cut surface inside the glass samples, which is expected to improve the water resistance of the coagulated surface. On the other hand, the O K-edge XANES spectra suggested that the O abundance in the coagulated surface layer was lower than that in the cut surface inside the glass samples, and that alkali metal elements may be concentrated in the coagulated surface layer. However, no difference was observed in the Na K-edge XANES spectra between the coagulated surface layer and the cut surface, and no difference was observed in the Si K-edge XANES spectra between the solidified surface and the inside of glass samples. In addition, the Ce L-edge XANES spectra confirmed that the Ce valence in the surface layer of coagulated glass samples were oxidized compared to the inside of glass samples.

Dissolution of zirconium-cerium oxide solid solution in an aqueous system

Kobayashi, Taishi*; Sato, Yutaro*; Tonna, Ryutaro*; Matsumura, Daiju; Sasaki, Takayuki*; Ikeda, Atsushi

Dalton Transactions (Internet), 53(46), p.18616 - 18628, 2024/10

https://doi.org/10.1039/D4DT02272F

Investigation of chemical state of uranium included in simulated waste glass

Katsuoka, Nanako; Akiyama, Daisuke*; Kirishima, Akira*; Nagai, Takayuki; Okamoto, Yoshihiro; Sato, Nobuaki*

2023-Nendo "Busshitsu, Debaisu Ryoiki Kyodo Kenkyu Kyoten" Kenkyu Seika, Katsudo Hokokusho (Internet), 1 Pages, 2024/07

no abstracts in English

Dissolution behavior and aging of iron-uranium oxide

Tonna, Ryutaro*; Sasaki, Takayuki*; Okamoto, Yoshihiro; Kobayashi, Taishi*; Akiyama, Daisuke*; Kirishima, Akira*; Sato, Nobuaki*

Journal of Nuclear Materials, 589, p.154862_1 - 154862_10, 2024/02

https://doi.org/10.1016/j.jnucmat.2023.154862

The dissolution behavior of FeUO compounds formed by a high-temperature reaction of UO with iron, a stainless-steel component of reactor structural materials, was investigated under atmospheric conditions. The compounds were prepared in an electric furnace using UO and FeO as starting materials, and their solid states were analyzed using X-ray diffraction, scanning electron microscopy energy dispersive X-ray spectroscopy, and X-ray absorption fine structure spectroscopy. The concentration of nuclides dissolved in water was examined by performing static leaching tests of FeUO compounds for up to three months. A redox reaction was proposed to occur between trivalent Fe and pentavalent U ions in the early stage of FeUO dissolution. It was thermodynamically deduced that the reduced divalent Fe ion was finally oxidized into a trivalent ion in the presence of dissolved oxygen, and iron hydroxide limited the solubility of Fe. Meanwhile, the concentration of hexavalent U (i.e., uranyl ion) was limited owing to the presence of secondary minerals such as metaschoepite and sodium uranate and subsequently decreased, possibly owing to sorption on Fe oxides, for example. The concentrations of multivalent ions of fission products, such as Ru and Ce, also decreased, likely for the reason above. By contrast, the concentration of soluble Cs ions did not decrease. The validity of this interpretation was supported by comparing the results with the dissolution behavior of a reference sample (Fe-free UO).

Structural investigation of borosilicate glasses by using XAFS measurement in soft X-ray region, 3 (Joint research)

Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Shibata, Daisuke*; Kojima, Kazuo*; Hasegawa, Takehiko*; Sato, Seiichi*; Fukaya, Akane*; Hatakeyama, Kiyoshi*

JAEA-Research 2023-004, 45 Pages, 2023/09

JAEA-Research-2023-004.pdf:6.07MB

The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, simulated waste glass samples were prepared and the chemical state regarding boron (B), silicon (Si) and waste elements of iron (Fe), cesium (Cs) were estimated by using XAFS measurement in soft X-ray region. To understand the chemical stability of simulated waste glasses, XANES spectra of B K-edge, Fe L, L-edge, and Cs M, M-edge were measured on the glass surface exposed to the leachate. As a result, it was found that the glass surface exposed to the leachate was changed and it was difficult to obtain a clear XANES spectrum. From the B K-edge XANES spectra on glass surfaces exposed to the leachate, an increase in three-coordination of B-O (BO) and a decrease in four-coordination of B-O (BO) were observed compared to the glass surfaces before immersion. The XANES spectra of Fe L, L-edge, and Cs M, M-edge show that as the exposure time in the leachate increases, the Cs present on the glass surface dissolves into the leachate. The XANES spectra of Si K-edge were measured on simulated waste glass surfaces before immersion, and it was confirmed that the change in XANES spectra given by NaO concentration had a larger effect than the waste component concentration.

Raman identification and characterization of chemical components included in simulated nuclear fuel debris synthesized from uranium, stainless steel, and zirconium

Kusaka, Ryoji; Kumagai, Yuta; Watanabe, Masayuki; Sasaki, Takayuki*; Akiyama, Daisuke*; Sato, Nobuaki*; Kirishima, Akira*

Journal of Nuclear Science and Technology, 60(5), p.603 - 613, 2023/05

https://doi.org/10.1080/00223131.2022.2128460

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.

End-to-end simulations and error studies of the J-PARC muon linac

Takeuchi, Yusuke*; Tojo, Junji*; Yamanaka, T.*; Nakazawa, Yuga*; Iinuma, Hiromi*; Kondo, Yasuhiro; Kitamura, Ryo; Morishita, Takatoshi; Cicek, E.*; Ego, Hiroyasu*; et al.

Proceedings of 31st International Linear Accelerator Conference (LINAC 2022) (Internet), p.562 - 564, 2022/10

https://doi.org/10.18429/JACoW-LINAC2022-TUPORI08

A muon linac is under development for future muon g-2/EDM experiments at J-PARC. The linac provides a 212 MeV muon beam to an MRI-type compact storage ring. After the initial acceleration using the electrostatic field created by mesh and cylindrical electrodes, the muons are accelerated using four types of radio-frequency accelerators. To validate the linac design as a whole, end-to-end simulations were performed using General Particle Tracer. In addition, error studies were performed to investigate the effects on beam and spin dynamics of various errors in the accelerator components and input beam distribution. This paper describes the results of the end-to-end simulations and error studies.

Structure, stability, and actinide leaching of simulated nuclear fuel debris synthesized from UO, Zr, and stainless-steel

Kirishima, Akira*; Akiyama, Daisuke*; Kumagai, Yuta; Kusaka, Ryoji; Nakada, Masami; Watanabe, Masayuki; Sasaki, Takayuki*; Sato, Nobuaki*

Journal of Nuclear Materials, 567, p.153842_1 - 153842_15, 2022/08

https://doi.org/10.1016/j.jnucmat.2022.153842

To understand the chemical structure and stability of nuclear fuel debris consisting of UO, Zr, and Stainless Steel (SUS) generated by the Fukushima Daiichi Nuclear Power Plant accident in Japan in 2011, simulated debris of the UO-SUS-Zr system and other fundamental component systems were synthesized and characterized. The simulated debris were synthesized by heat treatment for 1 to 12 h at 1600C, in inert (Ar) or oxidative (Ar + 2% O) atmospheres. Np and Am tracers were doped for the leaching tests of these elements and U from the simulated debris. The characterization of the simulated debris was conducted by XRD, SEM-EDX, Raman spectroscopy, and Mssbauer spectroscopy, which provided the major uranium phase of the UO -SUS-Zr debris was the solid solution of UO (s.s.) with Zr(IV) and Fe(II) regardless of the treatment atmosphere. The long-term immersion test of the simulated debris in pure water and that in seawater revealed the macro scale crystal structure of the simulated debris was chemically very stable in the wet condition for a year or more. Furthermore, the leaching test results showed that the actinide leaching ratios of U, Np, Am from the UO-SUS-Zr debris were very limited and less than 0.08 % for all the experiments in this study.

Stabilization treatment of nuclear fuel material contained with organic matter

Senzaki, Tatsuya; Arai, Yoichi; Yano, Kimihiko; Sato, Daisuke; Tada, Kohei; Ogi, Hiromichi*; Kawanobe, Takayuki*; Ono, Shimpei; Nakamura, Masahiro; Kitawaki, Shinichi; et al.

JAEA-Testing 2022-001, 28 Pages, 2022/05

JAEA-Testing-2022-001.pdf:2.33MB

In preparation for the decommissioning of Laboratory B of the Nuclear Fuel Cycle Engineering Laboratory, the nuclear fuel material that had been stored in the glove box for a long time was moved to the Chemical Processing Facility (CPF). This nuclear fuel material was stored with sealed by a polyvinyl chloride (PVC) bag in the storage. Since it was confirmed that the PVC bag swelled during storage, it seems that any gas was generated by radiolysis of the some components contained in the nuclear fuel material. In order to avoid breakage of the PVC bag and keep it safety for long time, we began the study on the stabilization treatment of the nuclear fuel material. First, in order to clarify the properties of nuclear fuel material, radioactivity analysis, component analysis, and thermal analysis were carried out. From the results of thermal analysis, the existence of organic matter was clarified. Then, ion exchange resin with similar thermal characteristics was selected and the thermal decomposition conditions were investigated. From the results of these analyzes and examinations, the conditions for thermal decomposition of the nuclear fuel material contained with organic matter was established. Performing a heat treatment of a small amount of nuclear fuel material in order to confirm the safety, after which the treatment amount was scaled up. It was confirmed by the weight change after the heat treatment that the nuclear fuel material contained with organic matter was completely decomposed.