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Yanagisawa, Kayo; Yokota, Hiromi*; Fujimoto, Katsushige*; Takagai, Yoshitaka*
Bunseki Kagaku, 73(9), p.515 - 522, 2024/09
On-line isotope dilution-laser ablation-inductively coupled plasma-mass spectrometry (on-line ID-LA-ICP-MS) is capable of quantification for each point ablated by laser, then the quantitative mapping of elements can be also conducted by reconstruction of the obtained each point data. The volume of data obtained as flow peaks in this system as a flow injection analysis, will be multiplied by each data such as number of m/z, scan time, time resolution and measurement position, and the total amount of data is enormous, resulting in a large human power and time consumption for data processing. In this paper, an original application software using Python to improve the efficiency of data processing in on-line ID-LA-ICP-MS was developed. To discriminate between the time-to-peak intensity and the background noise, an automatic peak detection using penalized asymmetric least squares was developed.
Matsueda, Makoto; Takagai, Yoshitaka*
Bunseki (Internet), 2024(6), p.195 - 200, 2024/06
The analytical demand for radioisotopes (RI) contained in radioactive waste from the decommissioning of nuclear power plants, research activities and nuclear accidents is increasing. However, traditional analytical methods of RI are mostly complicated and time-consuming, it is necessary to be rapid, simple and automatic methods. This paper describes the rapid analytical techniques of inductively coupled plasma-mass spectrometry in recent years, which current technology, challenges and perspective for the future.
Tomita, Jumpei; Tomita, Ryohei; Suzuki, Daisuke; Yasuda, Kenichiro; Miyamoto, Yutaka
Journal of the American Society for Mass Spectrometry, 35, p.1178 - 1183, 2024/05
A sensitive analytical technique was investigated in order to determine 10 order of U/U ratio in the sub-ng of uranium using a multi-collector ICP-MS. First, the solution volume was concentrated to one tenth to obtain higher intensities. Next, data acquisition was started from the beginning of the solution uptake and continued until all solution was exhausted. Taking advantage of multi-collector measurement, all data were used with excepting the portion affected by air mixing at the beginning and end of sample introduction. The isotope ratios were calculated from the total counts of each isotope. This technique was applied to U isotope standard (IRMM-184) to measure the 10 order of U/U ratio in the sub-ng of uranium. Measured values were in good agreement with the certified value within the uncertainity (=2). The uncertainties obtained with this new technique (32% on average) were revised to be 10 times smaller than those obtained with the conventionalmethod.
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.
Morii, Shiori; Yomogida, Takumi; Asai, Shiho*; Ouchi, Kazuki; Oka, Toshitaka; Kitatsuji, Yoshihiro
Bunseki Kagaku, 72(10.11), p.441 - 448, 2023/10
Rapid analytical method for the determination of Zr-93 in radioactive wastes has been developed. Laser ablation (LA)-ICP-MS was applied to the analysis of Zr isotopes in simulated high-level radioactive waste (HLW). Sample preparation time was dramatically reduced by using a DGA resin as the adsorbent for Zr. Direct quantification of Zr isotopes in this resin sample was carried out by LA-ICP-MS. Laser settings were optimized to obtain a reliable isotope ratio of the sample by LA-ICP-MS. Quantification of Zr isotopes in the simulated HLW solution by isotope dilution mass spectrometry (IDMS) was examined. The amount of Zr-90 in the sample obtained by IDMS corresponded to a value calculated from the given concentration of Zr in the sample within uncertainty. Thus, this method can be applied for the quantification of Zr-93 in radioactive wastes.
Yanagisawa, Kayo; Matsueda, Makoto; Furukawa, Makoto*; Ishiniwa, Hiroko*; Wada, Toshihiro*; Hirata, Takafumi*; Takagai, Yoshitaka*
Analyst, 148(18), p.4291 - 4299, 2023/09
Times Cited Count:0 Percentile:0.00(Chemistry, Analytical)Quantitative imaging of trace elements was successfully performed by online isotope dilution laser ablation inductively coupled plasma mass spectrometry (online LA-ICP-IDMS). The sample aerosols produced by LA are mixed online with the mist created from an isotopically enriched spike solution via an in-house cyclonic spray chamber, which has a gas port on the top. Quantification was continuously achieved in each spot; subsequently, quantitative imaging was realized. Fe and Sr were selected as the model elements, and their spot quantifications based on online-isotope dilution. The method was applied to actual biological hard tissues, and the results were compared with electron probe microanalyzer data.
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:1 Percentile:55.95(Chemistry, Analytical)Yuguchi, Takashi*; Ito, Daichi*; Yokoyama, Tatsunori; Sakata, Shuhei*; Suzuki, Satoshi*; Ogita, Yasuhiro; Yagi, Koshi*; Imura, Takumi*; Motai, Satoko*; Ono, Takeshi*
Lithos, 440-441, p.107026_1 - 107026_14, 2023/03
Times Cited Count:0 Percentile:0.02(Geochemistry & Geophysics)We propose a new method for elucidating zircon growth in granitic plutons, based on variations in three-dimensional 3D cathodoluminescence (CL) patterns, U-Pb ages, titanium concentration, and Th/U ratios. We focused on the zircon growth processes in the Okueyama granite (OKG) in central Kyushu, Japan, to obtain interpretations of magma chamber processes that result in the formation of granitic plutons. The OKG consists of three lithofacies: biotite granite (BG), hornblende granite (HG), and hornblende granodiorite (HGD). To determine the 3D internal structure and growth pattern of a zircon crystal, we performed CL observations for multi-sections of the samples. Simultaneously, we also determined the zircon U-Pb age and titanium concentration of the center sections of the samples. The 3D distribution of the oscillatory zoning can be used to determine the crystal nucleus. The simultaneous determination of zircon U-Pb ages and Ti concentrations of the granite samples indicates the time-temperature (t-T) history of granitic magma before its solidification. The t-T histories of the BG, HG, and HGD represented similar cooling behaviors within the magma chamber: rapid cooling from the zircon crystallization temperature to the closure temperature of the biotite K-Ar system between 16 Ma and 10 Ma. The variations in the Th/U ratios against temperature also demonstrate a different trend at the boundary of approximately 670 C. Fractional crystallization in the magma chamber progressed significantly at temperatures above 670 C; below 670 C, crystallization progressed slowly, indicating only minimal changes in the magma composition. The variations in the Th/U ratio against temperature in the BG, HG, and HGD portrayed common tendencies, indicating the same behavior in the progression of fractional crystallization among the three lithofacies, which in turn, represented the same behavior within the entire magma chamber.
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:48.47(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.
Matsueda, Makoto; Aoki, Jo; Koarai, Kazuma; Terashima, Motoki; Takagai, Yoshitaka*
Analytical Sciences, 38(11), p.1371 - 1376, 2022/11
Times Cited Count:3 Percentile:41.05(Chemistry, Analytical)The I analysis using ICP-MS is challenging caused by xenon-129 (Xe) and IH generated from excess stable isotope I. In this study, mass discrimination between iodine-129 (I) and interfering substances was achieved by inductively coupled plasma-tandem quadrupole mass spectrometry (ICP-MS/MS) with a dynamic reaction cell introduced a mixture gas of O and CO. As a result, the ratio of (background noise intensity at m/z 129)/I was 3.8 10 and 10 mBq/L of I was analyzed without chemical separation in the presence of 100 mg/L stable I. Spiked tests with actual rainwater were performed, and obtained values were agreed with the spiked amounts.
Koarai, Kazuma; Matsueda, Makoto; Terashima, Motoki
KEK Proceedings 2022-2, p.102 - 107, 2022/11
Analytical methods with inductively coupled plasm mass spectrometry (ICP-MS) have been developed for the determination of Sr in environmental samples; however, the sensitivity of the ICP-MS methods and removal of interferences are insufficient to measure trace amount of Sr in the environmental samples. In this study, we developed an analytical method for Sr with ICP-DRC-MS/MS using oxygen and ammonia mixed gas reaction. This analytical method could be applied for measurement of Sr in reference soil.
Yanagisawa, Kayo; Matsueda, Makoto; Furukawa, Makoto*; Takagai, Yoshitaka*
Analytical Sciences, 38(8), p.1105 - 1114, 2022/08
We demonstrate the sensitivity enhancement in inductively coupled plasma mass spectrometry (ICP-MS) by combining ultrasonic nebulization via the nitrogen mixed gas effect. We showed the effect of nitrogen gas concentration (0-5%) in the nebulizer gas on the signal sensitivity for 63 elements using commercially available (concentric and ultrasonic) nebulizers. In addition, the limit of detection was calculated in each case. Finally, we compared the sensitivity (i.e., the slope of the calibration curve), background noise intensity, and three-dimensional intensity distribution in the plasma to elucidate the effects of the concurrent use of mixed gas plasmas and nebulization methods.
Matsueda, Makoto; Kawakami, Tomohiko*; Koarai, Kazuma; Terashima, Motoki; Fujiwara, Kenso; Iijima, Kazuki; Furukawa, Makoto*; Takagai, Yoshitaka*
Chemistry Letters, 51(7), p.678 - 682, 2022/07
Times Cited Count:6 Percentile:63.27(Chemistry, Multidisciplinary)New methodology for a simultaneous isotope speciation of various Pu isotopes without complicated isobaric interferences is developed by using inductively coupled plasma-mass spectrometry (ICP-MS). In analyzing ICP tandem MS (ICP-MS/MS), CO gas reactions in a dynamic reaction cell (DRC) almost eliminated the background noise intensity produced by isobaric interference from isotopes originating from actinides such as Am, Cm, and U at the locations (m/z) of significant Pu isotopes (Pu, Pu, Pu, Pu, Pu).
Yuguchi, Takashi*; Yamazaki, Hayato*; Ishibashi, Kozue*; Sakata, Shuhei*; Yokoyama, Tatsunori; Suzuki, Satoshi*; Ogita, Yasuhiro; Sando, Kazusa*; Imura, Takumi*; Ono, Takeshi*
Journal of Asian Earth Sciences, 226, p.105075_1 - 105075_9, 2022/04
Times Cited Count:4 Percentile:54.83(Geosciences, Multidisciplinary)Simultaneous determination of the U-Pb age of zircon and concentration of titanium in a single analysis spot, using inductively coupled plasma mass spectrometry with laser ablation sample introduction, produces paired age and temperature data of zircon crystallisation, potentially revealing time-temperature () histories for evolved magma. The Kurobegawa granite, central Japan, contains abundant mafic magmatic enclaves (MMEs). We applied this method to evaluate MMEs and their host (enclosing) granites. Cooling behaviour common to both MMEs and host rocks was found between 1.5 and 0.5 Ma. Rapid cooling from the zircon crystallisation temperature to the closure temperature of biotite K-Ar system was within 1 million year. Combining the obtained paths of MMEs and host rocks with petrological information can provide insights into magma chamber processes. This suggests that MME flotation, migration, and spread through the magma chamber ceased at 1.5-0.5 Ma, indicating the emplacement age of the Kurobegawa granitic pluton, as no large-scale reheating episodes have occurred since then.
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.
Tomita, Jumpei; Ozawa, Mayumi; Ohara, Yoshiyuki; Miyamoto, Yutaka
KEK Proceedings 2021-2, p.130 - 134, 2021/12
no abstracts in English
Kagami, Saya; Yokoyama, Tatsunori; Umeda, Koji*
JAEA-Testing 2021-001, 49 Pages, 2021/08
To make a contribution to safety assessment for geological disposal of high level radioactive and/or TRU waste, we need to assess long-term stability of geological environment and predict long-term changes of geotectonic events that will occur in the future, especially for Quaternary period ( 2.6 million years ago-present). In the most case, we investigate chronological data of geological events by radiometric dating. When some geological samples have no objects to which radiometric dating method can be applied (e.g., zircon, biotite, wood fragments and plant residues), we can use tephrochronology, which is geological dating method using each layer of tephra (erupted volcanic ash), for dating of geological layers. This chronological method is essential in Japan, where volcanism is very active. Tephra is usually characterized by petrographic characteristics and/or chemical composition (mainly major elements) of volcanic glasses and/or minerals in tephra. In Tono Geoscience Center (Japan Atomic Energy Agency), we develop an analytical technique of chemical composition including trace elements of volcanic glasses for detailed tephra identification. In this paper, we report a sample preparation procedure and analytical methods of chemical compositions of individual volcanic glass shards by using an electron probe microanalyzer and a laser ablation-inductively coupled plasma-mass spectrometer.
Koarai, Kazuma; Matsueda, Makoto; Aoki, Jo; Yanagisawa, Kayo*; Terashima, Motoki; Fujiwara, Kenso; Kino, Yasushi*; Oka, Toshitaka; Takahashi, Atsushi*; Suzuki, Toshihiko*; et al.
Journal of Analytical Atomic Spectrometry, 36(8), p.1678 - 1682, 2021/08
Times Cited Count:5 Percentile:53.20(Chemistry, Analytical)Rapid analysis of Sr in bone and tooth samples of cattle were achieved by an inductively coupled plasma mass spectrometry (ICP-MS) coupled with mass shift and solid phase extraction techniques. Limit of detection (LOD) in the ICP-MS measurement of 0.1 g samples was lower than that of the radioactivity measurement. Analytical time of the ICP-MS method was reduced from 20 days to 11 hours, compared with the radiometric method. Therefore, the ICP-MS method can be rapid and useful procedure of Sr in small bone and tooth samples derived from terrestrial animals.
Matsueda, Makoto; Yanagisawa, Kayo*; Koarai, Kazuma; Terashima, Motoki; Fujiwara, Kenso; Abe, Hironobu; Kitamura, Akihiro; Takagai, Yoshitaka*
ACS Omega (Internet), 6(29), p.19281 - 19290, 2021/07
Times Cited Count:2 Percentile:13.70(Chemistry, Multidisciplinary)Online solid-phase extraction-inductively coupled plasma-quadrupole mass spectrometry with oxygen dynamic reaction cell (online SPE-ICP-MS-DRC) was shown to be a thorough automatic analytical system, circumventing the need for human handling. At three stepwise separations (SPE-DRC-Q mass filters), we showed that interference materials allowed the coexistence of abundance ratios of 1.510 for Tc/Mo. Using this optimized system, a detection limit of Tc was 9.3 pg/L (5.9 mBq/L) for a 50 mL injection and sequential measurements were undertaken at a cycle of 24 min/sample.