Development of a quantification method for Zr isotopes in solid samples by LA-ICP-MS for rapid analysis of Zr-93 in high-level radioactive wastes

Morii, Shiori; Yomogida, Takumi; Asai, Shiho*; Ouchi, Kazuki; Oka, Toshitaka; Kitatsuji, Yoshihiro

Bunseki Kagaku, 72(10.11), p.441 - 448, 2023/10

https://doi.org/10.2116/bunsekikagaku.72.441

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.

Reaction of Np, Am, and Cm ions with CO and O 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

https://doi.org/10.1039/D3JA00136A

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 …

Mass-spectrometric determination of iodine-129 using O-CO mixed-gas reaction in inductively coupled plasma tandem quadrupole mass spectrometry

Matsueda, Makoto; Aoki, Jo; Koarai, Kazuma; Terashima, Motoki; Takagai, Yoshitaka*

Analytical Sciences, 38(11), p.1371 - 1376, 2022/11

https://doi.org/10.1007/s44211-022-00180-w

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.

Using CO Reactions to Achieve Mass-spectrometric Discrimination in Simultaneous Plutonium-isotope Speciation with Inductively Coupled Plasma-Tandem Mass Spectrometry

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

https://doi.org/10.1246/cl.220160

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).

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.

Analytical method for chemical compositions of volcanic glasses in Tono Geoscience Center; Quantitative measurements of Major Elements by using EPMA and Minor Elements by LA-ICP-MS

Kagami, Saya; Yokoyama, Tatsunori; Umeda, Koji*

JAEA-Testing 2021-001, 49 Pages, 2021/08

JAEA-Testing-2021-001.pdf:3.86MB

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.

Online solid-phase extraction-inductively coupled plasma-quadrupole mass spectrometry with oxygen dynamic reaction for quantification of technetium-99

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

https://doi.org/10.1021/acsomega.1c02756

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.

Direct quantitation of Cs in spent Cs adsorbent used for the decontamination of radiocesium-containing water by laser ablation inductively coupled plasma mass spectrometry

Asai, Shiho*; Ohata, Masaki*; Hanzawa, Yukiko; Horita, Takuma; Yomogida, Takumi; Kitatsuji, Yoshihiro

Analytical Chemistry, 92(4), p.3276 - 3284, 2020/02

https://doi.org/10.1021/acs.analchem.9b05161

The long-term safety assessment of spent Cs adsorbents produced during the decontamination of radiocesium-containing water at the Fukushima Daiichi Nuclear Power Plant requires one to estimate their Cs content prior to final disposal. Cs is usually quantified by inductively coupled plasma mass spectrometry (ICP-MS), which necessitates the elution of Cs from Cs adsorbents. However, this approach suffers from the high radiation dose from Cs. To address this challenge, we herein employed laser ablation ICP-MS for direct quantitation of Cs in Cs adsorbents and used a model Cs adsorbent prepared by immersion of a commercially available Cs adsorbent into radiocesium-containing liquid waste to verify the developed technique. The use of the Cs/Cs ratio and Cs radioactivity obtained by gamma spectrometry achieved simple and precise quantitation of Cs and the resulting Cs activity of 0.36 Bq agreed well with that in the original radiocesium-containing liquid waste.

Rapid analytical method of Sr in urine sample; Rapid separation of Sr by phosphate co-precipitation and extraction chromatography, followed by determination by triple quadrupole inductively coupled plasma mass spectrometry (ICP-MS/MS)

Tomita, Jumpei; Takeuchi, Erina

Applied Radiation and Isotopes, 150, p.103 - 109, 2019/08

https://doi.org/10.1016/j.apradiso.2019.05.026

A rapid analytical method for determining Sr in urine samples (1-2 L) was developed to assess the internal exposure of workers in a radiological emergency. Strontium in a urine sample was rapidly separated by phosphate co-precipitation, followed by extraction chromatography with a tandem column of Pre-filter, TRU and Sr resin, and the Sr activity was determined by ICP-MS/MS. Measurement in the MS/MS mode with an O reaction gas flow rate 1 mL min showed no tailing of Sr at m/z = 90 up to 50 mg-Sr L. The interferences of Ge, Se and Zr at m/z = 90 were successfully removed by chemical separation. This analytical method was validated by the results of the analyses of synthetic urine samples (1.2-1.6 L) containing a known amount of Sr along with 1 mg of each of Ge, Se, Sr and Zr. The turnaround time for analysis was about 10 h, and the detection limit of Sr was approximately 1 Bq per urine sample.