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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:56.43(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$$^{-1}$$.

Journal Articles

Development of HCl-free solid phase extraction combined with ICP-MS/MS for rapid assessment of difficult-to-measure radionuclides, 1; Selective measurement of $$^{93}$$Zr and $$^{93}$$Mo in concrete rubble

Do, V. K.; Furuse, Takahiro; Murakami, Erina; Aita, Rena; Ota, Yuki; Sato, Soichi

Journal of Radioanalytical and Nuclear Chemistry, 327(1), p.543 - 553, 2021/01

 Times Cited Count:4 Percentile:58.27(Chemistry, Analytical)

A new HCl-free chromatographic separation procedure has been developed for sequential separation of Zr and Mo from concrete matrices. Accordingly, $$^{93}$$Zr and $$^{93}$$Mo could be sensitively and selectively measured by ICP-MS/MS using ammonia reaction gas. The recoveries of greater than 90% for Zr and Mo from concretes could be achieved. The measurement condition was optimized for complete suppression of interferences from $$^{93}$$Nb and peak tailing from abundant isotopes of Zr and Mo in concrete matrices. The removal of interferences was verified by measurement of radio-contamination-free concretes used as a sample matrix blank. Method detection limits of 1.7 mBq g$$^{-1}$$ and 0.2 Bq g$$^{-1}$$ were achieved for $$^{93}$$Zr and $$^{93}$$Mo, respectively, in the concrete matrices. The interference removal factor for Nb (equivalent to the decontamination factor in radiochemical separation) was of the order of 10$$^{5}$$, and the abundance sensitivity was of the order of 10$$^{-8}$$, indicating that the developed method is reliable for verifying the presence of ultralow concentrations of $$^{93}$$Zr and $$^{93}$$Mo. The present method is suitable for the rapid assessment of $$^{93}$$Zr and $$^{93}$$Mo for radioactivity inventory of concrete rubble.

JAEA Reports

Development of separation technique of Pu, Am, Np using solid phase extraction resin for the determination of impurity metal elements in plutonium nitrate solution by inductivity coupled plasma optical emission spectrometry

Taguchi, Shigeo; Yamamoto, Masahiko; Furuse, Takahiro*; Masaki, Yuji*; Kuno, Takehiko

JAEA-Technology 2018-005, 14 Pages, 2018/06

JAEA-Technology-2018-005.pdf:0.94MB

The method to remove Pu, Am and Np from plutonium nitrate solution recovered from spent nuclear fuel prior to ICP-OES measurement has been developed for the determination of 18 impurity metal elements (Fe, Cr, Ni, Mn, Al, Cd, V, Cu, Si, Zn, Mo, Sn, Ca, Mg, Na, Ag, Pb, B). In this method, two TRU resin packed columns were used for separation. In the first column, Pu and Am were mainly removed by adsorption. The recovered solution from the fist column was added to the second column after reduction of Np, and Am(III) and Np(IV) were removed by adsorption. The Pu nitrate solution (22g/L) of 2mL were treated by proposed method. The alpha emission nuclide was decreased to $$<$$5.8 Bq/mL in a solution diluted to 100mL. As a result of ICP-OES measurement, the recoveries of impurity metals separated by proposed method were almost 100%. This separation scheme can apply to the metal impurity elemental analysis in Pu nitrate solution recovered from spent nuclear fuel.

JAEA Reports

Determination of metal impurities in MOX powder by direct current arc atomic emission spectroscopy; Application of standard addition method for direct analysis of powder sample

Furuse, Takahiro*; Taguchi, Shigeo; Kuno, Takehiko; Surugaya, Naoki

JAEA-Technology 2016-028, 19 Pages, 2016/12

JAEA-Technology-2016-028.pdf:1.79MB

Metal impurities in MOX powder obtained from uranium and plutonium recovered from reprocessing process of spent nuclear fuel are needed to be determined for its characterization. Direct current arc atomic emission spectroscopy (DCA-AES) is one of the useful methods for direct analysis of powder sample without dissolving the analyte into aqueous solution. However, the selection of standard material, which can overcome concerns such as matrix matching, is quite important to create adequate calibration curves for DCA-AES. In this study, we apply standard addition method using the certified U$$_{3}$$O$$_{8}$$ containing known amounts of metal impurities to avoid the matrix problems. The proposed method provides good results for determination of Fe, Cr and Ni at a significant quantity level contained in MOX samples.

Oral presentation

Removal of alpha-ray emission nuclide from plutonium solution in reprocessing plant by solid phase extraction method for the analysis of metal impurities

Taguchi, Shigeo; Furuse, Takahiro*; Masaki, Yuji*; Inada, Satoshi; Takamura, Yuzuru*; Kuno, Takehiko

no journal, , 

The analytical procedure to separate from the impurity metals was established by adsorption of Pu and Am using TRU resin to analyze the impurity metal in Pu nitrate solution recovered from spent nuclear fuel.

Oral presentation

Development of an analytical method for nickel isotopes using an automated sample preparation system and ICP-QQQ-MS

Do, V. K.; Kitamura, Kiyoshi; Horita, Takuma; Furuse, Takahiro

no journal, , 

We report an application of automated devices for multi-step chemical separation for nickel and an idea of subsequent quantification for Ni-59 using ICP-QQQ-MS. Nickel is separated on our selected automated instruments applying a conventional separation scheme. The obtained chemical recovery for Ni standard carrier was 89.8% (relative standard deviation, RSD of 2.9%, n = 3), which is consistent with the manually obtained recovery of 87.0% (RSD = 2.2%, n = 3). The quantification of Ni-59 by ICP-QQQ-MS was examined. Accordingly, the intensity of 59Ni could be deduced from an intensity correction curve for natural isotopes of nickel. The proposed analytical method is more rapid and less laborious, being expected to reduce radiation exposure to workers.

Oral presentation

Annual outcomes Okuma Analysis and Research Center 2018

Furuse, Takahiro; Do, V. K.; Akutsu, Hideyuki; Horita, Takuma

no journal, , 

We will report status of development of analytical techniques and facilities for Okuma Analysis and Research Center as 2018 annual outcomes. In regard to development of analytical techniques, we will report rapid and efficient analytical methods for nuclides using ICP-MS and automated systems.

Oral presentation

Outline and construction status of Okuma Analysis and Research Center, Laboratory-1

Furuse, Takahiro; Ota, Yuki; Do, V. K.

no journal, , 

The Japan Atomic Energy Agency has been developing Okuma Analysis and Research Center, a research and development facility, in order to ascertain the properties of radioactive wastes and fuel debris towards the decommissioning of TEPCO's Fukushima Daiichi Nuclear Power Station (1F). In this presentation, we are reporting outline and construction status of Laboratory-1 which will analyse low and medium level samples in the Okuma Analysis and Research Center.

Oral presentation

Development of analytical methods for 1F-samples; Analysis of $$^{93}$$Zr by ICP-QQQ-MS and automated sample preparation instruments

Do, V. K.; Furuse, Takahiro; Ota, Yuki

no journal, , 

This presentation outlines our idea of method development for the analysis of $$^{93}$$Zr with application of ICP-QQQ-MS after a simple chemical separation using automated sample preparation instruments.

Oral presentation

Development of analytical methods for measurement of radioactive elements

Sato, Soichi; Do, V. K.; Furuse, Takahiro

no journal, , 

Oral presentation

Development of simultaneous analytical method for $$^{93}$$Zr and $$^{93}$$Mo based on solid phase extraction combined with ICP-MS/MS, 2; Spectral interference removal for measurement of $$^{93}$$Zr and $$^{93}$$Mo by ICP-MS/MS

Do, V. K.; Furuse, Takahiro; Murakami, Erina; Aita, Rena; Ota, Yuki; Tomitsuka, Tomohiro; Sano, Yuichi; Akimoto, Yuji*; Endo, Tsubasa*; Katayama, Atsushi; et al.

no journal, , 

The paper presents removal of possible interferences including from an isobar ($$^{93}$$Nb) and tailings of adjacent peaks for the quantification of $$^{93}$$Zr and $$^{93}$$Mo using an ICP-MS/MS (Agilent 8900). By using ammonia gas (NH$$_{3}$$) as a reaction gas, $$^{93}$$Zr and $$^{93}$$Mo can be separated from each other and from $$^{93}$$Nb owing to the different reactions of those elements with the reaction gas. Based on the characterization results, we propose a measurement scheme aiming at quantification of $$^{93}$$Zr and $$^{93}$$Mo in environmental samples collected at adjacent location of Fukushima Daiichi Nuclear Power Station.

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

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 HCl-free analysis method of $$^{113m}$$Cd using liquid scintillation counter

Ito, Chihiro; Tanaka, Yasuyuki; Kurosawa, Kiyoko*; Motoki, Yoshiaki*; Do, V. K.; Furuse, Takahiro

no journal, , 

In this presentation, an HCl-free analytical method for $$^{113m}$$Cd in aqueous solution samples containing multiple radionuclides by liquid scintillation counting is reported. We aimed to develop a chemical separation procedure of $$^{113m}$$Cd from co-existing nuclides such as $$^{60}$$Co and/or $$^{55}$$Fe, which interfere with the beta-counting. The use of hydrochloric acid (HCl) was avoided to prevent facilities from corrosion. Accordingly, after a sample-matrix separation with a chelating disk, Cd was adsorbed on a cation exchange resin and then selectively eluted by sodium thiosulfate (Na$$_{2}$$S$$_{2}$$O$$_{3}$$), which has a high affinity for Cd. This developed method allowed the separation and purification of Cd from the sample matrix without the use of halogen acids.

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.

21 (Records 1-20 displayed on this page)