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Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*
JAEA-Review 2023-025, 117 Pages, 2024/03
The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2022. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station (1F), Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2019, this report summarizes the research results of the "Development of extremely small amount analysis technology for fuel debris analysis" conducted in FY2022. Understanding the properties of fuel debris is necessary for handling, criticality control, storage control, etc. A key technique is the chemical analysis of actinide nuclides. We develop sample pretreatment technology and separation / analysis process required for chemical analysis. The purpose of this study is to streamline future planned fuel debris analysis. To promote 1F decommissioning, we will train human resources through on-the-job training.
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
Times Cited Count:0 Percentile:0.02(Chemistry, Analytical)Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*
JAEA-Review 2022-034, 135 Pages, 2023/01
The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2021. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station (1F), Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2019, this report summarizes the research results of the "Development of extremely small amount analysis technology for fuel debris analysis" conducted in FY2021. Understanding the properties of fuel debris is necessary for handling, criticality control, storage control, etc. A key technique is the chemical analysis of actinide nuclides. We develop sample pretreatment technology and separation / analysis process required for chemical analysis. The purpose of this study is to streamline future planned fuel debris analysis. To promote 1F decommissioning, we will train human resources through on-the-job training. In particular, we will apply the extremely small amount analysis (ICP-MS/MS), which has recently been successful …
Do, V. K.; Furuse, Takahiro; Ota, Yuki; Iwahashi, Hiroyuki; Hirosawa, Takashi; Watanabe, Masahisa; Sato, Soichi
Journal of Radioanalytical and Nuclear Chemistry, 331(12), p.5631 - 5640, 2022/12
Times Cited Count:2 Percentile:53.91(Chemistry, Analytical)Sn is one of the long-lived fission products that might have been released into the environment after the Fukushima nuclear accident in Japan in 2011. The presence of radionuclides must be monitored for the proper treatment of wastes obtained from decommissioning accident-related nuclear facilities and the surrounding environment. In the work, we propose a reliable method for verifying the presence of Sn in construction materials by combining the HCl-free solid phase extraction on TEVA resin and a selective measurement by inductively coupled plasma tandem mass spectrometry (ICP-MS/MS). The method has been optimized and characterized step by step. More than 95% of chemical recovery was achieved for Sn from typical concrete matrixes. The interference caused by an isobar Te and possible polyatomic interferences from matrixes were effectively suppressed by the developed chemical separation and the tandem MS/MS configuration. The total decontamination factor for the Te interference was of the order of 10. The estimated method detection limit for Sn in concrete as measured at m/z = 160 was 12.1 pg g, which is equivalent to 6.1 mBq g.
Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*
JAEA-Review 2021-056, 98 Pages, 2022/02
The Collaborative Laboratories for Advanced Decommissioning Science (CLADS), Japan Atomic Energy Agency (JAEA), had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project (hereafter referred to "the Project") in FY2020. The Project aims to contribute to solving problems in the nuclear energy field represented by the decommissioning of the Fukushima Daiichi Nuclear Power Station, Tokyo Electric Power Company Holdings, Inc. (TEPCO). For this purpose, intelligence was collected from all over the world, and basic research and human resource development were promoted by closely integrating/collaborating knowledge and experiences in various fields beyond the barrier of conventional organizations and research fields. The sponsor of the Project was moved from the Ministry of Education, Culture, Sports, Science and Technology to JAEA since the newly adopted proposals in FY2018. On this occasion, JAEA constructed a new research system where JAEA-academia collaboration is reinforced and medium-to-long term research/development and human resource development contributing to the decommissioning are stably and consecutively implemented. Among the adopted proposals in FY2019, this report summarizes the research results of the "Development of extremely small amount analysis technology for fuel debris analysis" conducted in FY2020. The fuel debris retrieved from the Fukushima Daiichi Nuclear Power Station (1F) is analyzed in the second building of the Okuma Analysis and Research Center. The characteristics of fuel debris, such as the mixture of nuclear fuel, reactor components, and concrete, are not clear, and its analysis will be the first attempt in the world. Understanding the properties of fuel debris is necessary for handling, criticality control, storage control, etc. A key technique is the chemical analysis of actinide nuclides. We develop sample pretreatment technology and separation/analysis process required for chemical analysis.
Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*
JAEA-Review 2020-064, 95 Pages, 2021/02
JAEA/CLADS had been conducting the Nuclear Energy Science & Technology and Human Resource Development Project in FY2019. Among the adopted proposals in FY2019, this report summarizes the research results of the "Development of extremely small amount analysis technology for fuel debris analysis" conducted in FY2019.
Tomita, Jumpei; Takeuchi, Erina
no journal, ,
no abstracts in English
Horita, Takuma; Akimoto, Yuji*; Kikuchi, Hikaru*; Do, V. K.
no journal, ,
no abstracts in English
Iwasaki, Maho; Suzuki, Tatsuya*; Yamamura, Tomoo*; Konashi, Kenji*; Shikamori, Yasuyuki*; Noguchi, Shinichi
no journal, ,
no abstracts in English
Horita, Takuma; Akimoto, Yuji*; Do, V. K.
no journal, ,
Samarium-151(Sm) can be measured by liquid scintillation counting (LSC) or inductively coupled plasma mass spectrometry (ICP-MS). While the former method requires a complete radiochemical separation, the latter one must solve the isobaric interference from Europium-151 (Eu). In this study, we have been developing an analytical technique for Sm by ICP-tandem MS(ICP-MS/MS). The recent advances of MS/MS mode with a collision/reaction cell in mass spectrometry may enable sufficient removal of the mass spectroscopic interferences. Moreover, compared to LSC, ICP-MS is more rapid and more selective, and thus, it can simplify pretreatment process. As preliminary experiments, the selection of reaction gas for the separation of Sm from Eu were examined by checking the product ions of Sm and Eu produced by reactions with the various gases (H, O, NH, and NO). Our obtained data showed that in the reaction with NH, Sm formed a product ion at mass shift of 16, while the reaction tendency of Eu is different. Accordingly, the counts of Sm and Eu at the mass shift of 16 were 9842 [cps/g/L] and 162 [cps/g/L], respectively. The difference in reactivity of Sm and Eu to NH gas can reduce interference of the Eu to the measurement of Sm.
Furuse, Takahiro; Do, V. K.; Aita, Rena; Ota, Yuki; Murakami, Erina; Tomitsuka, Tomohiro; Sano, Yuichi; Akimoto, Yuji*; Endo, Tsubasa*; Katayama, Atsushi; et al.
no journal, ,
In order to simplify the analysis of Zr and Mo in radioactive waste from conventional radiation measurement, we have considered analysis method combining solid-phase extraction and ICP-MS/MS. In this presentation, we report the results of a study on sequential chemical separation of Zr and Mo from Nb and sample matrix using ZR resin as a solid-phase extraction resin.
Ota, Yuki; Do, V. K.; Furuse, Takahiro; Sano, Yuichi; Iwahashi, Hiroyuki; Homma, Shunta; Ichijo, Yurina; Kurosawa, Kiyoko*; Endo, Tsubasa*; Motoki, Yoshiaki*; et al.
no journal, ,
no abstracts in English
Iwahashi, Hiroyuki; Do, V. K.; Furuse, Takahiro; Ota, Yuki; Homma, Shunta; Kurosawa, Kiyoko*; Motoki, Yoshiaki*; Hirosawa, Takashi
no journal, ,
The radiometric determination of beta emitting Pd (half-life of 6.5 million years) requires a multiple-step chemical separation and a time-consuming radioactive measurement. Inductively coupled plasma tandem mass spectrometry (ICP-MS/MS) with recent technological advances in interference removal by two quadrupole mass filters and a collision/reaction cell could be an alternative for highly sensitive analysis of long-lived radionuclides. In this study, we have developed an analytical method for the determination of Pd in concrete rubble by ICP-MS/MS combined with single-column chromatographic separation. A simplified procedure for the separation of Pd from concrete matrices was developed. The measurement condition was optimized to completely suppress the interference including the isobar Ag and the sample matrices. The application of the developed method to radioactive concrete rubble is under consideration.
Kazama, Hiroyuki; Sekio, Yoshihiro; Maeda, Koji; Konashi, Kenji*; Abe, Chikage*; Nagai, Yasuyoshi*; Suzuki, Tatsuya*
no journal, ,
Inductively coupled plasma mass spectrometry with triple quadrupoles (ICP-MS/MS) is one of the promising techniques for rapid and highly sensitive wet analysis of fuel debris in Fukushima Daiichi Nuclear Power Plant. The collision/reaction cell technology implanted in ICP-MS/MS is available option to eliminate isobaric interferences, being expected to simplify the pretreatment of fuel debris analysis. In this study, ICP-MS/MS measurements of U and Th with collision/reaction gases were performed. On the basis of their gas reactivity, analytical methods for U will be discussed.
Kazama, Hiroyuki; Sekio, Yoshihiro; Maeda, Koji; Koyama, Shinichi; Suzuki, Tatsuya*; Konashi, Kenji*; Abe, Chikage*; Nagai, Yasuyoshi*
no journal, ,
Triple-quadrupole inductively coupled plasma mass spectrometry (ICP-MS/MS) is an attractive technique to perform rapid and highly sensitive analysis. The collision/reaction cell (CRC) technology incorporated in ICP-MS/MS is an available option to eliminate isobaric interference, being expected to discriminate actinide nuclides involved in fuel debris. Meanwhile, in order to discriminate against these isobaric interferences using ICP-MS/MS, it is necessary to understand actinide gas-phase reaction behavior associated with the injection of reaction gases into the CRC. In the present work, the actinide molecular ion formations correlating with the excitation energy from the ground state of actinide monoatomic cation to their reactive state (5f6d) were investigated by injection of reaction gases into CRC. The obtained correlations allow us to predict the reaction behaviors towards mutual discrimination of actinide series using ICP-MS/MS.
Banjarnahor, I. M.; Do, V. K.; Motoki, Yoshiaki*; Ota, Yuki; Iwahashi, Hiroyuki; Kurosawa, Kiyoko*; Furuse, Takahiro
no journal, ,
Pure beta-emitting Se is one of the long-lived fission products that might release to the environment due to the nuclear accident at Fukushima Daiichi Nuclear Power Plant (FDNPP). A reliable and simple determination method of the radionuclide is important for proceeding the disposal of the wastes obtained from the decommissioning of FDNPP. We developed a new analytical procedure for the measurement of Se by inductively coupled plasma triple quadrupole mass spectrometry (ICP-MS/MS). All interferences that potentially interfere in the measurement of Se could be effectively removed by the chemical separation pretreatment and ICP-MS/MS. The method is tested with inactive concrete to verify the interference removal efficiency. Also, the analytical figures of merit such as detection capability etc. are reported.
Tanaka, Yasuyuki; Do, V. K.; Motoki, Yoshiaki*; Ota, Yuki; Iwahashi, Hiroyuki; Kurosawa, Kiyoko*; Furuse, Takahiro
no journal, ,
We examined the measurement method of U using triple-quadrupole inductively coupled plasma-mass spectrometry (ICP-MS/MS, Agilent 8900). The measurable mass to charge ratio (m/z) is expanded up to 275, the device can measure UOO (m/z = 268) generated by the reaction with O, which was used as a reaction gas. This mass shift mode decreased the interference from hydride of U compared to the previously reported analytical method, which improved limit of detection of U using ICP-MS/MS. In this presentation, the optimized measurement condition of U measured at m/z = 268 by ICP-MS/MS is reported.
Ota, Yuki; Kurosawa, Kiyoko*; Motoki, Yoshiaki*; Do, V. K.; Furuse, Takahiro
no journal, ,
We have developed an analytical method of I (half-life: 1.57x10 years) and Cl (half-life: 3.01x10 years) in various radioactive rubbles generated by decommissioning of the Fukushima Daiichi Nuclear Power Plant (1F). A sequential chemical separation procedure has been developed to isolate the nuclides from the sample matrix, followed by the quantification by inductively coupled plasma-mass spectrometry (ICP-MS/MS) and liquid scintillation counting (LSC), respectively.
Do, V. K.; Ota, Yuki; Banjarnahor, I. M.; Aita, Rena; Murakami, Erina; Homma, Shunta; Iwahashi, Hiroyuki; Furuse, Takahiro
no journal, ,
The Okuma Analysis and Research Center has been established to analyze the decommissioning wastes collected from Fukushima Daiichi Nuclear Power Plant (1F). Radioactive material analysis and research facility 1 (Laboratory-1) where analyses of the low and intermediate-level wastes are preliminarily tested has started the operation from October 2022. Among the selected radionuclides to be analyzed, long-lived radionuclides can be measured by inductively coupled plasma mass spectrometry, which offers more rapid measurement and higher sensitivity compared to radiometry. The modern configuration of tandem triple quadrupoles (called ICP-QQQ-MS or ICP-MS/MS) enables the effective control of interferences that can simplify the chemical separation process and thus reduces the total time of analysis. The presentation summarizes our recent advances in research and development of analytical methods for the selected long-lived radionuclides such as Zr, Mo, Pd, Sn, and Se by ICP-MS/MS, aiming at applications to the measurement of samples collected in the vicinity of 1F. The analytical method development and recently obtained results are discussed in detail.
Matsueda, Makoto
no journal, ,
no abstracts in English