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
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.
Kazama, Hiroyuki; Konashi, Kenji*; Suzuki, Tatsuya*; Koyama, Shinichi; Maeda, Koji; Sekio, Yoshihiro; Onishi, Takashi; Abe, Chikage*; Shikamori, Yasuyuki*; Nagai, Yasuyoshi*
Journal of Analytical Atomic Spectrometry, 38(8), p.1676 - 1681, 2023/07
Nagai, Yuya; Shuji, Yoshiyuki; Kawasaki, Takeshi; Aita, Takahiro; Kimura, Yasuhisa; Nemoto, Yasunori*; Onuma, Takeshi*; Tomiyama, Noboru*; Hirano, Koji*; Usui, Yasuhiro*; et al.
JAEA-Technology 2022-039, 117 Pages, 2023/06
Japan Atomic Energy Agency (JAEA) manages wide range of nuclear facilities. Many of these facilities are required to be performed adjustment with the aging and complement with the new regulatory standards and the earthquake resistant, since the Great East Japan Earthquake and the Fukushima Daiichi Nuclear Power Station accident. It is therefore desirable to promote decommissioning of facilities that have reached the end of their productive life in order to reduce risk and maintenance costs. However, the progress of facility decommissioning require large amount of money and radioactive waste storage space. In order to address these issues, JAEA has formulated a "The Medium/Long-Term Management Plan of JAEA Facilities" with three pillars: (1) consolidation and prioritization of facilities, (2) assurance of facility safety, and (3) back-end countermeasures. In this plan, Plutonium Fuel Fabrication Facility has been selected as primary decommissioned facility, and dismantling of equipment in the facilities have been underway. In this report, size reduction activities of the glove box W-9 and a part of tunnel F-1, which was connected to W-9, are presented, and the obtained findings are highlighted. The glovebox W-9 had oxidation & reduction furnace, and pellet crushing machine as equipment interior. The duration of activity took six years from February 2014 to February 2020, including suspended period of 4 years due to the enhanced authorization approval process
Oba, Yojiro; Motokawa, Ryuhei; Kaneko, Koji; Nagai, Takayuki; Tsuchikawa, Yusuke; Shinohara, Takenao; Parker, J. D.*; Okamoto, Yoshihiro
Scientific Reports (Internet), 13, p.10071_1 - 10071_8, 2023/06
Nagai, Yuki; Shinaoka, Hiroshi*
Journal of the Physical Society of Japan, 92(3), p.034703_1 - 034703_8, 2023/03
no abstracts in English
Nagai, Yuki; Tanaka, Akinori*; Tomiya, Akio*
Physical Review D, 107(5), p.054501_1 - 054501_16, 2023/03
no abstracts in English
JAEA-Research 2022-014, 84 Pages, 2023/02
Most of the simulated waste glasses used for physical property evaluation are processed into a shape suitable for the measurement method from glass gob obtained by slowly cooling molten glass to room temperature. However, the actual vitrified waste glass material is obtained by cooling and being coagulated the glass drained from the bottom of glass melter into the canister. In this study, Raman spectroscopy was performed on the coagulated surface of molten simulated waste glass in the depth direction to evaluate the state of the Si-O bridging structure near the coagulated glass surface. The Raman spectra measured from the surface to the depth direction near the surface of the glasses produced by several melting and coagulation conditions of molten simulated waste glass cullet in the air atmosphere, and it was confirmed that there were changes in these spectra. On the other hand, the raw material glass cullet and the surface of the glass solidified in argon gas atmosphere showed little change in the spectrum in the depth direction, and the Si-O bridging structure near the glass surface was similar. It was also confirmed that the spectrum change in the depth direction measurement was small for the cut surface of the glass, and that the change in the spectrum for the broken glass fracture surface was also small. For glasses with a large change in Raman spectra in the depth direction near the coagulated surface, the molten glass was cooled from the molten state to room temperature in a muffle furnace with air atmosphere. That is, the magnitude of the spectral change with respect to the depth direction depends on the time from the molten state to coagulation. In order to confirm the reason why the number of bridging oxygen in the Si-O bridging structure is small on the coagulated surface of glass, the XANES spectra of Si-K edge and Ce-L3 edge were measured by XAFS on the coagulated surface and the cutting face. As a result, the Si-K edge peak on the coagulated surface is
Wallerberger, M.*; Badr, S.*; Hoshino, Shintaro*; Huber, S.*; Kakizawa, Fumiya*; Koretsune, Takashi*; Nagai, Yuki; Nogaki, Kosuke*; Nomoto, Takuya*; Mori, Hitoshi*; et al.
Software X (Internet), 21, p.101266_1 - 101266_7, 2023/02
no abstracts in English
Nagai, Takayuki; Tone, Masaya; Katsuoka, Nanako; Okamoto, Yoshihiro; Baba, Yuji*; Akiyama, Daisuke*
Photon Factory Activity Report 2022 (Internet), 3 Pages, 2023/00
no abstracts in English
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
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.
Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
JAEA-Research 2022-008, 37 Pages, 2022/10
The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, borosilicate glass frit and 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. Following results were obtained by XAFS measurements of simulated waste glass surfaces after immersion test to investigate the long chemical stability. (1) As the leaching time of glass samples in immersion test passed, the Cs M, M-edge XANES spectra disappeared and the Fe L, L-edge spectra changed. (2) A new compound was formed on the sample surface after the immersion test, and these changes in the surface state were confirmed by Raman spectroscopy. However, it became difficult to obtain a clear B K-edge XANES spectrum by forming a compound on glass surfaces. The Si K-edge XANES spectra of borosilicate glass frits with different NaO content were measured, and following was confirmed. (1) As the NaO concentration increases in borosilicate glass frit, the K-edge peak of Si shifts to the low energy side. (2) The intensity of the Si K-edge peak is maximum when the NaO content in glass frits was about 7wt%.
Nakayama, Hiromasa; Onodera, Naoyuki; Satoh, Daiki; Nagai, Haruyasu; Hasegawa, Yuta; Idomura, Yasuhiro
Journal of Nuclear Science and Technology, 59(10), p.1314 - 1329, 2022/10
We developed a local-scale high-resolution atmospheric dispersion and dose assessment system (LHADDAS) for safety and consequence assessment of nuclear facilities and emergency response to nuclear accidents or deliberate releases of radioactive materials in built-up urban areas. This system is composed of pre-processing of input files, main calculation by local-scale high-resolution atmospheric dispersion model using large-eddy simulation (LOHDIM-LES) and real-time urban dispersion simulation model based on a lattice Boltzmann method (CityLBM), and post-processing of dose-calculation by simulation code powered by lattice dose-response functions (SIBYL). LHADDAS has a broad utility and offers superior performance in (1) simulating turbulent flows, plume dispersion, and dry deposition under realistic meteorological conditions, (2) performing real-time tracer dispersion simulations using a locally mesh-refined lattice Boltzmann method, and (3) estimating air dose rates of radionuclides from air concentrations and surface deposition in consideration of the influence of individual buildings and structures. This system is promising for safety assessment of nuclear facilities as an alternative to wind tunnel experiments, detailed pre/post-analyses of a local-scale radioactive plume dispersion in case of nuclear accidents, and quick response to emergency situations resulting from deliberate release of radioactive materials by a terrorist attack in an urban central district area.
Isegawa, Kazuhisa; Setoyama, Daigo*; Higuchi, Yuki*; Matsumoto, Yoshihiro*; Nagai, Yasutaka*; Shinohara, Takenao
Nuclear Instruments and Methods in Physics Research A, 1040, p.167260_1 - 167260_10, 2022/10
Akiyama, Daisuke*; Kusaka, Ryoji; Kumagai, Yuta; Nakada, Masami; Watanabe, Masayuki; Okamoto, Yoshihiro; Nagai, Takayuki; Sato, Nobuaki*; Kirishima, Akira*
Journal of Nuclear Materials, 568, p.153847_1 - 153847_10, 2022/09
FeUO, CrUO, and FeCrUO are monouranates containing pentavalent U. Even though these compounds have similar crystal structures, their formation conditions and thermal stability are significantly different. To determine the factors causing the difference in thermal stability between FeUO and CrUO, their crystal structures were evaluated in detail. A Raman band was observed at 700 cm in all the samples. This Raman band was derived from the stretching vibration of the O-U-O axis band, indicating that FeCrUO was composed of a uranyl-like structure in its lattice regardless of its "x"' value. Mssbauer measurements indicated that the Fe in FeUO and FeCrUO were trivalent. Furthermore, FeCrUO lost its symmetry around Fe with increasing electron densities around Fe, as the abundance of Cr increased. These results suggested no significant structural differences between FeUO and CrUO. Thermogravimetric measurements for UO, FeUO, and CrUO showed that the temperature at which FeUO decomposed under an oxidizing condition (approximately 800 C) was significantly lower than the temperature at which the decomposition of CrUO started (approximately 1250 C). Based on these results, we concluded that the decomposition of FeUO was triggered by an "in-crystal" redox reaction, i.e., Fe U Fe U, which would not occur in the CrUO lattice because Cr could never be reduced under the investigated condition. Finally, the existence of Cr in FexCrUO effectively suppressed the decomposition of the FeCrUO crystal, even at a very low Cr content.
Physical Review B, 106(6), p.064506_1 - 064506_10, 2022/08
no abstracts in English
Julia Programming for Numerical Computation; A One-week Course, 244 Pages, 2022/06
no abstracts in English
Nagai, Yasuki*; Kawabata, Masako*; Hashimoto, Shintaro; Tsukada, Kazuaki; Hashimoto, Kazuyuki*; Motoishi, Shoji*; Saeki, Hideya*; Motomura, Arata*; Minato, Futoshi; Ito, Masatoshi*
Journal of the Physical Society of Japan, 91(4), p.044201_1 - 044201_10, 2022/04
Recently, Lu is considered as one of the most important medical RIs for treating neuroendocrine tumors. A plan to produce Lu with high purity by using enriched Yb samples with irradiation of deuteron beams in accelerators has been discussed. However, since the other Yb isotopes contained in the Yb sample interacts with deuterons, Lu isotopes other than Lu are produced as impurities. Since the purity of Lu is important for medical use, a method to evaluate the impurity of Lu has been required. In this study, we proposed a new method to estimate production yields of each Lu isotopes in Yb samples with arbitrary isotopic compositions by using excitation functions of Yb()Lu reactions and the particle transport calculation code PHITS. The method plays an important role in discussing the isotopic composition of enriched samples to produce high-purity Lu using accelerators.
Motokawa, Ryuhei; Kaneko, Koji; Oba, Yojiro; Nagai, Takayuki; Okamoto, Yoshihiro; Kobayashi, Taishi*; Kumada, Takayuki; Heller, W. T.*
Journal of Non-Crystalline Solids, 578, p.121352_1 - 121352_7, 2022/02
Nagai, Takayuki; Okamoto, Yoshihiro; Yamagishi, Hirona*; Ota, Toshiaki*; Kojima, Kazuo*; Inose, Takehiko*; Sato, Seiichi*; Hatakeyama, Kiyoshi*
JAEA-Research 2021-010, 62 Pages, 2022/01
The local structure of glass-forming elements and waste elements in borosilicate glasses varies with its chemical composition. In this study, borosilicate glass frit and simulated waste glass samples were prepared and the local structure and chemical state regarding boron(B), oxygen(O), silicon(Si) and waste elements of iron(Fe), cesium(Cs) were estimated by using XAFS measurement in soft X-ray region. Following results were obtained by XAFS measurements of prepared glass frit and simulated waste glass samples: (1) The effect of NaO concentration on B-O coordination structure is greater than that of the waste elements concentration. (2) The height of pre-edge by O K-edge spectrum depends on the concentration of first transition elements such as Fe in glass samples. Following results were obtained by XAFS measurements of simulated waste glass samples after immersion test to investigate the long chemical stability. (1) A new compound was formed on the sample surface after the immersion test, and changes in the surface state were confirmed by Raman spectroscopy. (2) Cs on the sample surface after immersion test dissolves into the leaching solution. The Si K-edge XANES spectra of borosilicate glass frits and simulated waste glass samples included lanthanides oxide were measured, and following was confirmed. (1) As the NaO concentration increases in borosilicate glass frit, the K-edge peak of Si shifts to the low energy side. (2) The peak height of the K-edge of Si differs depending on the kind of lanthanide.