Recent progress of Cs concentration and Cs/Cs isotopic ratio measurement

Shimada, Asako

Bunseki Kagaku, 71(12), p.625 - 633, 2022/12

https://doi.org/10.2116/bunsekikagaku.71.625

Cesium-135 is one of the important nuclides to assess the safe disposal of High Level Waste (HLW). Therefore, the calculation code and library to evaluate the Cs concentration in HLW have been improved through comparisons with experimental results. On the other hand, even basic data of Cs, such as its half-life, have large uncertainty. Because the Cs/Cs isotopic ratio suggests its origin and introduction date, the ratios in environmental samples are measured to study global fallout from nuclear weapons testing and nuclear accidents. Such measurement methods was attracted attention, in particular, after the accident at the Fukushima Daiichi Nuclear Power Station. Measurement of the Cs/Cs isotopic ratio in environmental samples was challenging because the radiocesium has a very low concentration and it co-exists with huge amounts of Ba isotopes, which are isobaric interfering nuclides, are co-exist. Chemical separation methods were developed to eliminate interfering nuclides and improve the performance of the mass spectrometer to enable the measurement of the ratios. In this review, the features of the Cs/Cs isotopic ratio for each origin and recent developments in measurement techniques are summarized.

Determination of Cs/Cs isotopic ratio in soil collected near Fukushima Daiichi Nuclear Power Station through mass spectrometry

Shimada, Asako; Tsukahara, Takehiko*; Nomura, Masao*; Kim, M. S.*; Shimada, Taro; Takeda, Seiji; Yamaguchi, Tetsuji

Journal of Nuclear Science and Technology, 58(11), p.1184 - 1194, 2021/11

https://doi.org/10.1080/00223131.2021.1931520

Determining the completeness of nuclear reactor decommissioning is an important step in safely utilizing nuclear power. For example, Cs from the Fukushima Daiichi Nuclear Power Station (FDNPS) accident can be treated as background radioactivity, so determining the origin of Cs is essential. To accomplish this, measuring the Cs/Cs isotope ratio can be useful, so this study optimized a solvent extraction method, with calix[4]arene-bis(t-octylbenzo-crown-6) [BOBCalixC6] in 1-octanol, to purify radioactive Cs, radiocesium, from a solution of major environmental soil elements and mass spectrometry interference elements. This optimized method was applied to Cs purification in soil samples (40 g), and the final solutions contained a total of 10g/ml of the major soil elements and ng/ml concentrations at most of interfering elements. Soil samples collected near the FDNPS were then purified, and the Cs/Cs isotope ratios were measured, using both thermal ionization mass spectrometry (TIMS) and triple quadrupole induced coupled plasma mass spectrometry (ICP-QQQ). The results of each of these measurements were compared, and we found that Cs isotope ratios obtained by TIMS were more precise, by an order of magnitude, while the ICP-QQQ results possessed good abundance sensitivities. A slightly higher Cs/Cs ratio in the northwest area of the FDNPS was observed, while other areas exhibited similar values, all within the measurement error range, which indicated different origins of radiocesium. These results agreed with previously reported Cs/Cs activity distributions, suggesting that this ratio may be useful in identifying radiocesium origins for evaluating future nuclear reactor decommissions.

Appreciate new century award

Shimada, Asako

Nihon Bunseki Kagakukai Kanto Shibu Nyusu, (31), p.7 - 8, 2021/00

I am very glad to win a prize, new century award of Kanto branch of The Japan Society for Analytical Chemistry. I deeply appreciate recommender and co-workers. The title of award was "Development of analytical method of difficult to measure nuclides in radioactive wastes", and especially development of analytical method for Am-242m, Mo-93, and I-129 was recognized. By measuring beta-ray of Am-242, which is progeny nuclide of Am-242m and having high intensity and shorter half-life, measuring time was shortened to approximately 1/20 compare to traditional method. Analyzed Mo-93 example was extremely few. When Mo-93 was analyzed via X-ray, Zr-93 and Nb-93m were the interfering nuclides, therefore, separation method of Mo from Zr and Nb was developed and the method was applied to the rubble sample collected at the Fukushima Daiichi Nuclear Power Station (FDNPS). Official method to measure I-129 in environmental samples were optimized to measure I-129 in the contaminated water collected at FDNPS.

Sensitivity analysis of external exposure dose for future burial measures of decontamination soil generated outside Fukushima prefecture

Shimada, Asako; Sawaguchi, Takuma; Takeda, Seiji

Proceedings of 2020 International Conference on Nuclear Engineering (ICONE 2020) (Internet), 5 Pages, 2020/08

https://doi.org/10.1115/ICONE2020-16826

no abstracts in English

Dose estimation for contaminated soil storage in living environment

Takai, Shizuka; Shimada, Asako; Sawaguchi, Takuma; Takeda, Seiji; Kimura, Hideo

Radiation Protection Dosimetry, 188(1), p.1 - 7, 2020/01

https://doi.org/10.1093/rpd/ncz250

After the Fukushima Nuclear Power Plant accident, most of radiocesium-contaminated soil generated from decontamination activities outside Fukushima prefecture has been stored at decontamination sites such as schools, parks and residential lands (storage at sites) according to the Decontamination Guidelines. However, additional exposure due to the present storage has not been evaluated. Moreover, entering storage sites, which is not restricted for storage at sites, was not considered in safety assessment conducted in the guidelines. To continue the storage and confirm the effectiveness, understanding of present possible exposures is important. In this study, we evaluated exposure doses for residents and users of storage sites based on the present situation. As a result, annual doses due to residence were 10 to 10 mSv y and doses due to annual entries were of the order of 10 mSv y. Hence, we confirmed that the exposure due to present storage outside Fukushima is significantly less than 1 mSv y.

Report of participation in Radiochemical Conference

Shimada, Asako

Hosha Kagaku, (38), p.30 - 31, 2018/09

no abstracts in English

Development of Zr, Mo, Pd and Sn analytical methods for radioactive waste from Fukushima Daiichi Nuclear Power Station

Aono, Ryuji; Sato, Yoshiyuki; Shimada, Asako; Tanaka, Kiwamu; Ueno, Takashi; Ishimori, Kenichiro; Kameo, Yutaka

JAEA-Technology 2017-025, 32 Pages, 2017/11

JAEA-Technology-2017-025.pdf:1.45MB

We have developed analytical methods for Zr, Mo, Pd and Sn, which are considered important in terms of the safety assessment of radioactive waste disposal. The methods are specialized for the wastes left after Fukushima accident. As the main analytical sample, we assumed accumulated water / treated water collected at Fukushima Daiichi Nuclear Power Station. As for Zr, Mo, Pd and Sn contained in this accumulated water / treated water, we have worked on the development of separation and purification method of target nuclide and improvement of recovery, and summarized these results in this report.

Separation of Zr in the rubble waste generated at the Fukushima Daiichi Nuclear Power Station

Shimada, Asako; Kameo, Yutaka

Journal of Radioanalytical and Nuclear Chemistry, 311(3), p.1613 - 1618, 2017/03

AA2016-0191.pdf:0.23MB

https://doi.org/10.1007/s10967-016-5126-5

Separation method of Zr using trans uranium resin (TRU resin) was developed. Approximately 100% of Zr, Nb, Bi, Th, and U and a part of Mo and Hg were extracted on the TRU resin from 3 M HNO solution and separated from Li, Be, Mg, Al, Ca, V, Cr, Mn, Fe, Co, Ni, Cu, Zn, Ga, As, Se, Rb, Sr,Ag, Cd, In, Cs, Ba. Approximately 100% of Zr, Nb, and U were striped from the TRU resin with 0.01 M HF and 10% of Mo, 7.1% of Hg, 77% of Bi, and 20% of Th were also included in the stripping solution. In order to measure Zr with inductively coupled plasma mass spectrometry (ICP-MS), Zr has to be separated from Nb and Mo to avoid isobaric interference. Therefore, further purification of Zr using tetra valent actinide resin (TEVA resin) was applied. The developed method was evaluated with the simulated rubble sample solution. Although a part of Zr was eluted during sample loading, most of Zr was extracted on the TRU resin and separated major elements of the rubble sample. Finally, Zr was separated from Nb and Mo with the TEVA resin.

Analysis of the radioactivity concentrations in low-level radioactive waste generated from JPDR facilities, 4

Omori, Hiroyuki; Nebashi, Koji; Shimada, Asako; Tanaka, Kiwamu; Yasuda, Mari; Hoshi, Akiko; Tsuji, Tomoyuki; Ishimori, Kenichiro; Kameo, Yutaka

JAEA-Data/Code 2014-029, 31 Pages, 2015/03

JAEA-Data-Code-2014-029.pdf:1.51MB

Simple and rapid methods to evaluate the radioactivity concentrations are required for the radioactive waste generated from research facilities in the Japan Atomic Energy Agency to dispose of in a near-surface repository. In order to establish the methods to evaluate the radioactivity concentrations of miscellaneous solid waste generated from research and testing reactors, we collected and analyzed samples from miscellaneous solid waste generated by the decommissioning of JPDR (Japan Power Demonstration Reactor). In this report, we reported the analytical data determined in fiscal 2014 (Cs and Mo) and summarized them with the radioactivity concentrations obtained in the past as basic data to consider the evaluation method of radioactivity concentrations in the stored waste taken from JPDR.

Development of a rapid analytical method for I in the contaminated water and tree samples at the Fukushima Daiichi Nuclear Power Station

Shimada, Asako; Ozawa, Mayumi; Kameo, Yutaka; Yasumatsu, Takuyo*; Nebashi, Koji*; Niiyama, Takuya; Seki, Shuhei; Kajio, Masatoshi; Takahashi, Kuniaki

Nuclear Back-end and Transmutation Technology for Waste Disposal, p.311 - 317, 2015/00

https://doi.org/10.1007/978-4-431-55111-9_27

no abstracts in English