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Yoneyama, Kai; Nitta, Ayako; Tanaka, Yasuyuki; Kodaka, Noriyasu; Kikuchi, Riku; Sakano, Takuma; Furuse, Takahiro; Sato, Soichi; Sambongi, Mitsuru; Tanaka, Kosuke
JAEA-Technology 2025-008, 44 Pages, 2025/12
JAEA-Technology-2025-008.pdf:4.3MB
At the TEPCO's Fukushima Daiichi Nuclear Power Station (1F), an investigation inside the reactors has been carried out. In order to safely carry out the decommissioning work such as fuel debris retrieval and building demolition, it is important to estimate the contamination in primary containment vessel for control the decommissioning planning and the worker radiation exposure levels. Therefore, the analysis of the deposit inside the penetration for the 1F Unit 2 primary containment vessel ("X-6 penetration") was performed to clarify the components and activity. The smears from the deposit were used for the analysis. Non-destructive analysis such as gamma-ray spectrometry, X-ray Fluorescence (XRF) and Scanning Electron Microscope-Energy dispersive X-ray spectroscopy (SEM-EDX) for the smear-samples were performed to determine the gamma-nuclides and the morphology of elements in the deposit. Furthermore, in order to evaluate the nuclides and nuclide composition of the deposit in detail, the smear-samples were dissolved and the quantitative analysis of gamma-nuclides, Sr-90, alpha-nuclides in the dissolved solution were conducted. The results (non-destructive analysis and quantitative analysis) were compared with the results of samples collected at different locations in the X-6 penetration in 2020. In the gamma-ray spectrometry as non-destructive analysis where the smears were analyzed directly, Co-60, Sb-125, Cs-134, Cs-137, Eu-154, Eu-155 and Am-241 were detected. In XRF results, Fe originating from construction material was detected as a major element and small amount of U and Zr originating from the fuel and fuel cladding were also detected. In SEM-EDX results, O and Fe were found as a major element of the deposit and U particles coexisting with Fe, Si, Cr, Ni and Zr were also found. These results were consistent with the SEM-EDX results of the samples collected in 2020. In radioactivity analysis, quantitative values for gamma-nuclides (Co-60, Sb-125, Cs-134, Cs-137, Eu-154, Eu-155), Sr-90, Pu-238, Pu-239+240, Am-241, Cm-244, U-235 and U-238 were obtained. Using the results, the ratios of radioactivity based on Cs-137 and U-238 were calculated. Both sets of the ratios were compared to the calculated value of the Unit 2 fuel composition from ORIGEN.
Se concentration in concrete rubbleBanjarnahor, I. M.; Do, V. K.; Furuse, Takahiro; Ota, Yuki; Tanaka, Kosuke
Journal of Radioanalytical and Nuclear Chemistry, 10 Pages, 2025/00
Times Cited Count：0 Percentile：73.02(Chemistry, Analytical)
Sn in concrete rubbleDo, 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：5 Percentile：53.41(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.
Zr and Mo in concrete rubbleDo, 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：7 Percentile：66.24(Chemistry, Analytical)A new HCl-free chromatographic separation procedure has been developed for sequential separation of Zr and Mo from concrete matrices. Accordingly, Zr and 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 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 and 0.2 Bq g were achieved for Zr and 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, and the abundance sensitivity was of the order of 10
, indicating that the developed method is reliable for verifying the presence of ultralow concentrations of Zr and Mo. The present method is suitable for the rapid assessment of Zr and Mo for radioactivity inventory of concrete rubble.
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.
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
O
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.
古瀬 貴広; 雛 哲郎
鳴海 昭紀*; 盛田 和久*
JP, 2020-089874 Patent licensing information Patent publication (In Japanese)
【課題】加工屑を高い回収率で回収できる集塵ドリル装置を提供する。 【解決手段】ドリル本体10が、先端にドリルチップ11を有するリード部12と、リード部12に連結される連結部15と、リード部12の先端から連結部15の外周面15Aに接続される貫通孔16,17と、を有し、ドリルチップ11が、リード部12より外径が大きく構成され、密閉体20が貫通穴25と、被加工物Mに設置される設置面26と、設置面26の反対側の非設置面27と、貫通穴25と接続する連結孔28と、を有する本体21と、非設置面27に設けられ連結部15と同じ径又は小さい径の孔23Aを有し気密性を有する材質で構成された第1弾性体23と、を有し、ドリル本体10が、孔23Aを貫通して被加工物Mに当接するように構成され、連結孔28とフィルター30が気密性を保持して接続された集塵ドリル装置1を提供する。
Zr and Mo based on solid phase extraction combined with ICP-MS/MS, 2; Spectral interference removal for measurement of Zr and Mo by ICP-MS/MSDo, 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 (Nb) and tailings of adjacent peaks for the quantification of Zr and Mo using an ICP-MS/MS (Agilent 8900). By using ammonia gas (NH) as a reaction gas, Zr and Mo can be separated from each other and from 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 Zr and Mo in environmental samples collected at adjacent location of Fukushima Daiichi Nuclear Power Station.
Zr and Mo based on solid phase extraction combined with ICP-MS/MS, 1; Sequential chemical separation of Zr and Mo from NbFuruse, 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 Zr and 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.
Pd in radioactive rubbles by ICP-MS/MSIwahashi, Hiroyuki; Do, V. K.; Furuse, Takahiro; Ota, Yuki; Homma, Shunta; Kurosawa, Kiyoko*; Motoki, Yoshiaki*; Hirosawa, Takashi
no journal, ,
The radiometric determination of beta emitting 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 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 Ag and the sample matrices. The application of the developed method to radioactive concrete rubble is under consideration.
Se in concrete by ICP-MS/MSBanjarnahor, I. M.; Do, V. K.; Motoki, Yoshiaki*; Ota, Yuki; Iwahashi, Hiroyuki; Kurosawa, Kiyoko*; Furuse, Takahiro
no journal, ,
Pure beta-emitting 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 Se by inductively coupled plasma triple quadrupole mass spectrometry (ICP-MS/MS). All interferences that potentially interfere in the measurement of 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.
Cd using liquid scintillation counterIto, Chihiro; Tanaka, Yasuyuki; Kurosawa, Kiyoko*; Motoki, Yoshiaki*; Do, V. K.; Furuse, Takahiro
no journal, ,
In this presentation, an HCl-free analytical method for Cd in aqueous solution samples containing multiple radionuclides by liquid scintillation counting is reported. We aimed to develop a chemical separation procedure of Cd from co-existing nuclides such as 
Co and/or 
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
SO), 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.
U using ICP-MS/MSTanaka, Yasuyuki; Do, V. K.; Motoki, Yoshiaki*; Ota, Yuki; Iwahashi, Hiroyuki; Kurosawa, Kiyoko*; Furuse, Takahiro
no journal, ,
We examined the measurement method of 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 U
OO (m/z = 268) generated by the reaction with O, which was used as a reaction gas. This mass shift mode decreased the interference from hydride of 
U compared to the previously reported analytical method, which improved limit of detection of U using ICP-MS/MS. In this presentation, the optimized measurement condition of U measured at m/z = 268 by ICP-MS/MS is reported.
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 Zr, Mo, Pd, Sn, and 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.
Se in concrete rubble by ICP-MS/MSDo, V. K.; Banjarnahor, I. M.; Ota, Yuki; Tanaka, Yasuyuki; Furuse, Takahiro; Tanaka, Kosuke
no journal, ,
The presentation summarizes the results of the development of analytical method for Se in concrete rubble using inductively coupled plasma triple quadrupole mass spectrometry (ICP-MS/MS). Se has been conventionally measured by a liquid scintillation counter (LSC). However, LSC measurement is time-consuming and susceptible to the radioactive interferences from highly radioactive nuclides (
Sr, 
Cs, etc.) coexisting in the samples. In this regard, ICP-MS/MS is a powerful technique, which can effectively eliminate the interferences. In this study, we have developed an HCl-free chemical separation to recover Se and remove the Br isobar. Chemical recovery for Se was around 90%. Also, we investigated the best conditions to measure Se by ICP-MS/MS. The method detection limit of 0.1 Bq/g was achieved indicating that the developed method meets the requirements for the measurement of Se in the radioactive rubble collected at the Fukushima Daiichi Nuclear Power Plant.
Furuse, Takahiro
no journal, ,
For conducting a large amount of analysis for rubble generated by the accident, new rapid and easy analysis methods have been developed in Okuma Analysis and Research Center. In this presentation, outline of the analysis technology and achievements using the technology in this fiscal year is reported.
Nitta, Ayako; Aita, Rena; Furuse, Takahiro; Tanaka, Kosuke
no journal, ,
no abstracts in English
Tanaka, Yasuyuki; Nitta, Ayako; Ota, Yuki; Kikuchi, Riku; Iwai, Tenga; Kodaka, Noriyasu; Aita, Rena; Sakano, Takuma; Furuse, Takahiro; Tanaka, Kosuke
no journal, ,
no abstracts in English
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 Sn by mass spectrometer.
Sn in radioactive rubbles by ICP-MS/MSOta, 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
