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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$$^{-1}$$.

Oral presentation

Development of chemical separation of Sn from concrete matrices using TEVA resin

Do, V. K.; Furuse, Takahiro; Ota, Yuki; Sano, Yuichi; Iwahashi, Hiroyuki; Homma, Shunta; Ichijo, Yurina; Kurosawa, Kiyoko*; Endo, Tsubasa*; Motoki, Yoshiaki*; et al.

no journal, , 

This paper presents an HCl-free chemical separation procedure for Sn recovery from concretes. Two pretreatment methods of solution samples followed by a proposed solid-phase extraction on TEVA resin were examined. The obtained results show that Sn can be highly recovered by the developed separation scheme with good reproducibility. The developed method is aimed at practical application to purification of Sn from concrete rubble for quantification of $$^{126}$$Sn by mass spectrometer.

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 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

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.

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