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Journal Articles

Reaction of Np, Am, and Cm ions with CO$$_{2}$$ and O$$_{2}$$ in a reaction cell in triple quadrupole inductively coupled plasma mass spectrometry

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

JAEA Reports

Development of extremely small amount analysis technology for fuel debris analysis (Contract research); FY2021 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*

JAEA-Review 2022-034, 135 Pages, 2023/01

JAEA-Review-2022-034.pdf:8.5MB

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 …

Journal Articles

Development of HCl-free solid phase extraction combined with ICP-MS/MS for rapid assessment of difficult-to-measure radionuclides, 2; Highly sensitive monitoring of $$^{126}$$Sn in concrete rubble

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:0 Percentile:59.27(Chemistry, Analytical)

$$^{126}$$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 $$^{126}$$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 $$^{126}$$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$$^{5}$$. The estimated method detection limit for $$^{126}$$Sn in concrete as measured at m/z = 160 was 12.1 pg g$$^{-1}$$, which is equivalent to 6.1 mBq g$$^{-1}$$.

JAEA Reports

Development of extremely small amount analysis technology for fuel debris analysis (Contract research); FY2020 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*

JAEA-Review 2021-056, 98 Pages, 2022/02

JAEA-Review-2021-056.pdf:9.08MB

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.

JAEA Reports

Development of extremely small amount analysis technology for fuel debris analysis (Contract research); FY2019 Nuclear Energy Science & Technology and Human Resource Development Project

Collaborative Laboratories for Advanced Decommissioning Science; Tohoku University*

JAEA-Review 2020-064, 95 Pages, 2021/02

JAEA-Review-2020-064.pdf:9.48MB

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.

Oral presentation

Rapid determination of $$^{90}$$Sr in urine samples by extraction chromatography coupled to ICP-MS/MS

Tomita, Jumpei; Takeuchi, Erina

no journal, , 

no abstracts in English

Oral presentation

Development of analytical techniques of $$^{93}$$Zr and $$^{93}$$Mo in fuel debris by ICP-MS/MS

Horita, Takuma; Akimoto, Yuji*; Kikuchi, Hikaru*; Do, V. K.

no journal, , 

no abstracts in English

Oral presentation

Fundamental study for analysis of Np-237 by ICP-MS/MS

Iwasaki, Maho; Suzuki, Tatsuya*; Yamamura, Tomoo*; Konashi, Kenji*; Shikamori, Yasuyuki*; Noguchi, Shinichi

no journal, , 

no abstracts in English

Oral presentation

Development of rational analytical technique of $$^{151}$$Sm by ICP-MS/MS

Horita, Takuma; Akimoto, Yuji*; Do, V. K.

no journal, , 

Samarium-151($$^{151}$$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 ($$^{151}$$Eu). In this study, we have been developing an analytical technique for $$^{151}$$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 $$^{151}$$Sm from $$^{151}$$Eu were examined by checking the product ions of $$^{147}$$Sm and $$^{151}$$Eu produced by reactions with the various gases (H$$_{2}$$, O$$_{2}$$, NH$$_{3}$$, and N$$_{2}$$O). Our obtained data showed that in the reaction with NH$$_{3}$$, Sm formed a product ion at mass shift of 16, while the reaction tendency of Eu is different. Accordingly, the counts of $$^{147}$$Sm and $$^{151}$$Eu at the mass shift of 16 were 9842 [cps/$$mu$$g/L] and 162 [cps/$$mu$$g/L], respectively. The difference in reactivity of Sm and Eu to NH$$_{3}$$ gas can reduce interference of the $$^{151}$$Eu to the measurement of $$^{151}$$Sm.

Oral presentation

Development of simultaneous analytical method for $$^{93}$$Zr and $$^{93}$$Mo based on solid phase extraction combined with ICP-MS/MS, 1; Sequential chemical separation of Zr and Mo from Nb

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 $$^{93}$$Zr and $$^{93}$$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.

Oral presentation

Removal of interferences for ultrasensitive detection of $$^{126}$$Sn in radioactive rubbles by ICP-MS/MS

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

Oral presentation

Interference removal for high-sensitivity rapid analysis of $$^{107}$$Pd in radioactive rubbles by ICP-MS/MS

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 $$^{107}$$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 $$^{107}$$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 $$^{107}$$Ag and the sample matrices. The application of the developed method to radioactive concrete rubble is under consideration.

Oral presentation

Development of ultramicro analysis technology for fuel debris analysis, 5; Consideration of analytical methods for actinide elements with ICP-MS/MS

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 $$^{238}$$U and $$^{232}$$Th with collision/reaction gases were performed. On the basis of their gas reactivity, analytical methods for U will be discussed.

Oral presentation

Prediction of gas-phase reactivity of actinide ions using triple quadrupole ICP-MS for fuel debris analysis

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 (5f$$^{n-2}$$6d$$^{2}$$) 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.

Oral presentation

Development of analytical method for interference-free determination of $$^{79}$$Se in concrete by ICP-MS/MS

Banjarnahor, I. M.; Do, V. K.; Motoki, Yoshiaki*; Ota, Yuki; Iwahashi, Hiroyuki; Kurosawa, Kiyoko*; Furuse, Takahiro

no journal, , 

Pure beta-emitting $$^{79}$$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 $$^{79}$$Se by inductively coupled plasma triple quadrupole mass spectrometry (ICP-MS/MS). All interferences that potentially interfere in the measurement of $$^{79}$$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.

Oral presentation

Development of measurement method of $$^{236}$$U using ICP-MS/MS

Tanaka, Yasuyuki; Do, V. K.; Motoki, Yoshiaki*; Ota, Yuki; Iwahashi, Hiroyuki; Kurosawa, Kiyoko*; Furuse, Takahiro

no journal, , 

We examined the measurement method of $$^{236}$$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 $$^{236}$$U$$^{16}$$O$$^{16}$$O (m/z = 268) generated by the reaction with $$^{16}$$O, which was used as a reaction gas. This mass shift mode decreased the interference from hydride of $$^{235}$$U compared to the previously reported analytical method, which improved limit of detection of $$^{236}$$U using ICP-MS/MS. In this presentation, the optimized measurement condition of $$^{236}$$U measured at m/z = 268 by ICP-MS/MS is reported.

Oral presentation

Development of analytical method of $$^{129}$$I and $$^{36}$$Cl for radioactive rubbles

Ota, Yuki; Kurosawa, Kiyoko*; Motoki, Yoshiaki*; Do, V. K.; Furuse, Takahiro

no journal, , 

We have developed an analytical method of $$^{129}$$I (half-life: 1.57x10$$^{7}$$ years) and $$^{36}$$Cl (half-life: 3.01x10$$^{5}$$ 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.

Oral presentation

Interference-free determination for long-lived radionuclides based on solid-phase extraction combined with ICP-MS/MS

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 $$^{93}$$Zr, $$^{93}$$Mo, $$^{107}$$Pd, $$^{126}$$Sn, and $$^{79}$$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.

Oral presentation

Development of rapid and easy analytical method for difficult-to-measure radionuclides

Matsueda, Makoto

no journal, , 

no abstracts in English

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