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.

Physical property investigation of gloves for glove boxes in nuclear fuel reprocessing plants; Physical properties of used gloves and estimation of its life-time

Yamamoto, Masahiko; Nishida, Naoki; Kobayashi, Daisuke; Nemoto, Ryo*; Hayashi, Hiroyuki*; Kitao, Takahiko; Kuno, Takehiko

JAEA-Technology 2023-004, 30 Pages, 2023/06

JAEA-Technology-2023-004.pdf:1.94MB

Glove-box gloves, that are used for handling nuclear fuel materials at the Tokai Reprocessing Plant (TRP) of the Japan Atomic Energy Agency, have an expiration date by internal rules. All gloves are replaced at a maximum of every 4-year. However, degrees of glove deterioration varies depending on its usage environment such as frequency, chemicals, and radiation dose. Therefore, physical properties such as tensile strength, elongation, hardness of gloves are measured and technical evaluation method for the glove life-time is established. It was found that gloves without any defects in its appearance have enough physical properties and satisfies the acceptance criteria values of new gloves. Thus, it was considered that the expired gloves could be used for total of 8-year, by adding 4-year of new glove life-time. In addition, the results of extrapolation by plotting the glove's physical properties versus the used years showed that the physical properties at 8-year is on the safer side than the reported physical properties of broken glove. Also, the data are not significantly different from the physical properties of the long-term storage glove (8 and 23 years). Based on these results, life-time of gloves at TRP is set to be 8-year. The frequency of glove inspections are not changed, and if any defects is found, the glove is promptly replaced. Thus, the risk related to glove usage is not increased. The cost of purchasing gloves, labor for glove replacement, and the amount of generated waste can be reduced by approximately 40%, respectively, resulting in more efficient and rationalized glove management.

Development of training course on non-destructive assay of nuclear material for Asian region, 2; Development of lectures and exercises on gamma-ray measurement

Yamamoto, Masahiko; Kono, Soma; Saegusa, Yu; Kuno, Takehiko; Sekine, Megumi; Inoue, Naoko; Noro, Naoko; Rodriguez, D.; Yamaguchi, Tomoki; Stinett, J.*

Proceedings of INMM & ESARDA Joint Annual Meeting 2023 (Internet), 10 Pages, 2023/05

The gamma-ray measurement part of the Non-Destructive Assay (NDA) course of safeguards and nuclear material accountancy was developed to focus on gamma-ray measurement allotting two days out of five days. The lectures on the basic characteristics and detection methods and mechanism of gamma-ray detectors were provided as e-learnings which were developed. The part for hands-on exercises were implemented in JAEA facility. Participants have set up each gamma-ray detector, and performed measurements of uranium and the other gamma-ray emitting nuclides. Also, uranium-235 enrichment measurements have been performed. In addition, the participants trained with a handheld gamma-ray spectrometer, HM-5, that is popular for IAEA safeguards as the preparation in the measurement exercise of fresh fuel assemblies in JRR-3, a research reactor facility of JAEA. This paper reports on the development, implementation, and feedback from participants on gamma-ray measurement part of the NDA course.

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.

Completion of waste removal work from the hot cell of Operation Testing Laboratory in Tokai Reprocessing Plant

Goto, Yuichi; Suzuki, Yoshimasa; Horigome, Kazushi; Miyamoto, Toshihiko*; Usui, Masato*; Mori, Eito*; Kuno, Takehiko

JAEA-Technology 2022-005, 42 Pages, 2022/07

JAEA-Technology-2022-005.pdf:4.48MB

Radioactive wastes were generated and stored in the hot cell of Operation Testing Laboratory of Tokai Reprocessing Plant due to the experiments related to the reprocessing technology development from 1974 to 2014. Waste removal work was strengthened by the shift work in the past, however another wastes were generated by the equipment dismantling. From 2006, an improved waste removal method was established by using bag-out technique and wastes were taken from the glove-box connected to the hot cell. The removal period, estimated from the conventional method using Cask No. 10, was reduced from 14 to 5 years. From 2016, upgrade of worker's awareness including related departments was performed by various software and hardware improvements. Also, the worker's skills were improved and equipment in Cask No.10 was checked for preventive maintenance. The prevention measures for past troubles were discussed with Radiation Control Department. In addition, transportation schedule including safety operation with Transportation Department and Waste Receiving Department was optimized to maintain the waste removal cycle. The removal period was reduced from 5 to 3 years by the above efforts. Finally, the work was completed in March 2020.

Investigation of physical properties of glove for glove-box and estimation of its life-time

Kobayashi, Daisuke; Yamamoto, Masahiko; Nishida, Naoki; Miyoshi, Ryuta; Nemoto, Ryo*; Hayashi, Hiroyuki*; Kato, Keisuke; Nishino, Saki; Kuno, Takehiko; Kitao, Takahiko; et al.

Nihon Hozen Gakkai Dai-18-Kai Gakujutsu Koenkai Yoshishu, p.237 - 240, 2022/07

All gloves attached to glove-box in Tokai Reprocessing Plant have a fixed expiration date and have to be replaced every 4-year. However, degrees of glove deterioration are different depending on its usage environment (frequency, chemicals, radiation, etc.), because of rubber products. Therefore, physical properties such as tensile strength, elongation, hardness of gloves are measured, and the life-time of gloves are estimated. As a result, gloves without any defects in its appearance have enough physical property for acceptance criteria of new glove. The extrapolated physical property of glove is sufficiently larger than the reported values of damaged glove. No deterioration in physical properties of gloves, that are periodically replaced without any defects in its appearance, is observed and the usable life-time of the glove is estimated to be 8 years.

Design of microchannel suitable for packing with anion exchange resins; Uranium separation from seawater containing a large amount of cesium

Ouchi, Kazuki; Tsukahara, Takehiko*; Brandt, A.*; Muto, Yuki*; Nabatame, Nozomi*; Kitatsuji, Yoshihiro

Analytical Sciences, 37(12), p.1789 - 1794, 2021/12

https://doi.org/10.2116/analsci.21P110

We attempted to scale down a separation process of uranium (U) using the microchip column loaded with anion exchange resin to develop safety and waste-reducing separation technique. The ideal separation performance of U was obtained by the properly design of a microchannel. The concentration of U in seawater as a real-world sample could be quantified with the prepared microchip column. It indicates that the microchip column is sufficiently practical. Compared to separation of U with a general column, the column size was successfully scaled down to 1/5000.

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.

Survey on the radioactive substance in the coastal areas near Fukushima Prefecture in FY2019 (Contract research)

Misono, Toshiharu; Tsuruta, Tadahiko; Nakanishi, Takahiro; Sanada, Yukihisa; Shiribiki, Takehiko; Miyamoto, Kenji*; Urabe, Yoshimi*

JAEA-Research 2020-008, 166 Pages, 2020/10

JAEA-Research-2020-008.pdf:13.11MB
JAEA-Research-2020-008(errata).pdf:0.92MB

After the accident at TEPCO Fukushima Daiichi Nuclear Power Station (1F), marine monitoring survey on radioactive substances have been conducted with financially supported by the Nuclear Regulatory Agency from FY2019. Results obtain in the project in FY2019 are presented in this report. Based on scientific grounds, the concept necessary for "progress of sea area monitoring" was arranged for the future medium- to long-term investigation of radiocesium concentrations. As basic information of survey frequency revise, a seabed topography and sediment distribution survey was conducted, and an attempt was made to understand the relationship between the seabed topography and the grain size distribution of bottom sediment. A columnar core sample was collected in the coastal area and analyzed for radioactive cesium concentration. In order to understand the dynamics of radioactive cesium contained in suspended matter flowing in from a river, suspended solids was collected using a sediment trap and the concentration of radioactive cesium was measured. We re-analyzed the towed monitoring data that had been implemented since 2013, and tried to improve the accuracy of the radioactive cesium distribution estimation map in the coastal area.

Automation technique of analytical pre-treatment for radioactive sample measurement using the program written by visual basic for applications

Yamamoto, Masahiko; Karo, Yoshinori*; Kodaka, Noriyasu; Kuno, Takehiko

JAEA-Technology 2019-014, 68 Pages, 2019/10

JAEA-Technology-2019-014.pdf:2.93MB

Analytical devices like syringe pump, electric burette, fraction collector, and electric valve have been controlled by the program written with Visual Basic for Applications (VBA Macro) to automate the column separation of radioactive sample measurement. It is found that VBA Macro can control each device. Therefore, automatic conditioning and separation equipment were made by combining each device and sequentially controlling with the program. The automation conditioning equipment can repeatedly perform conditioning operation with maximum of 8 columns. The automation separation equipment can separate and recover Sr in simulated highly active liquid waste by using Eichrom Technologies Sr resin. It is found that the developed automation method, using commercially available VBA Macro, is effective to reduce labor work, operator's radiation exposure, and to prevent operational error of analysis, together with reducing the cost of automation.