Asai, Shiho*; Ohata, Masaki*; Hanzawa, Yukiko; Horita, Takuma; Yomogida, Takumi; Kitatsuji, Yoshihiro
Analytical Chemistry, 92(4), p.3276 - 3284, 2020/02
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.
Fujiwara, Kenso; Yanagisawa, Kayo*; Iijima, Kazuki
Environmental Radiochemical Analysis VI, p.89 - 96, 2019/09
Since Strontium-90 (Sr-90) is one of the high yield and hazardous fission products, accurate and low-level detection of Sr-90 is essential for environmental samples. Especially, in case of nuclear power plant accidents, rapid and precise assessment of Sr-90 for environmental monitoring and health physics is required. In order to evaluate the migration of radionuclides in the environment, not only Sr-90 in water but also those in soil and biological samples should be measured. A new method for rapid quantification of Sr-90 by online solid phase extraction coupled with inductively coupled plasma mass spectrometry (SPE-ICP-MS) has been developed. In this method, it is unavoidable to eliminate the interference by polyatomic ion (e.g., ArCa, Ca) induced by isotopes and matrices in fishes and soil. In this study, SPE-ICP-MS method was applied to the measurement of Sr-90 in fishes, and the influence of the Sr isotopes and coexisting ions such as Ca was evaluated.
Tomita, Jumpei; Takeuchi, Erina
Applied Radiation and Isotopes, 150, p.103 - 109, 2019/08
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.
Bunseki, 2019(3), p.112 - 113, 2019/03
no abstracts in English
Asai, Shiho; Ohata, Masaki*; Yomogida, Takumi; Saeki, Morihisa*; Oba, Hironori*; Hanzawa, Yukiko; Horita, Takuma; Kitatsuji, Yoshihiro
Analytical and Bioanalytical Chemistry, 411(5), p.973 - 983, 2019/02
Determination of radiopalladium Pd is required for ensuring the radiation safety of Pd extracted from spent nuclear fuel for recycling or disposal. We employed laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS) to simplify an analytical procedure of Pd. Pd was separated through selective Pd precipitation reaction from spent nuclear fuel. Laser ablation allows direct measurement of the Pd precipitates, skipping the dissolution and dilution procedure. In this study, Pd in natural Pd standard solution was used as an internal standard, taking advantage of its absence in spent nuclear fuel. The Pd precipitate was uniformly embedded on the surface of the centrifugal filter, forming a microscopically thin flat surface of Pd. The resulting homogeneous Pd layer is suitable for obtaining a stable signal ratio of Pd/Pd. The amount of Pd obtained by LA-ICP-MS corresponds to the values obtained by conventional solution nebulization measurement.
Bunko Kenkyu, 67(6), p.239 - 240, 2018/12
A spectroscopic technique for analysis developed by collaboration between Japan Atomic Energy Agency (JAEA) and Quantum and Radiological Science and Technology (QST) is discussed for readers outside the field of nuclear energy. This paper introduces a quantitative analysis for Pd radioisotope contained in a spent nuclear fuel by using laser-induced photoreduction and inductively coupled plasma mass spectrometry (ICP-MS). The importance and problems of quantitative analysis for radioisotopes in spent nuclear fuels are described, and the principle, advantages, and future applications of the spectroscopic technique are discussed.
Yokoyama, Tatsunori; Kimura, Junichi*; Mitsuguchi, Takehiro; Danhara, Toru*; Hirata, Takafumi*; Sakata, Shuhei*; Iwano, Hideki*; Maruyama, Seiji*; Chang, Q.*; Miyazaki, Takashi*; et al.
Geochemical Journal, 52(6), p.531 - 540, 2018/12
Yomogida, Takumi; Asai, Shiho; Saeki, Morihisa*; Hanzawa, Yukiko; Horita, Takuma; Esaka, Fumitaka; Oba, Hironori*; Kitatsuji, Yoshihiro
Bunseki Kagaku, 66(9), p.647 - 652, 2017/09
Palladium-107 is a long-lived fission product, which can be found in high-level radioactive liquid wastes (HLLW). Determination of the Pd contents in HLLW is essential to evaluate the long-term safety of HLLW repositories. However, the Pd content in HLLW has not been reported because of difficulties in pretreatment for the measurement. In this study, we investigated applicability of laser-induced photoreduction to HLLW solution: it enables a simple and non-contact separation of Pd. The results showed the recovery of 60% was achieved at the conditions: 40% ethanol, 20 min irradiation, 100 mJ of pulse energy. Additionally, major radionuclides and potentially interfering components in ICP-MS were removed from the simulated HLLW over a wide concentration range of Pd from 0.24 to 24 mg L, showing the applicability of the proposed separation technique to HLLW samples.
Asai, Shiho; Saito, Kyoichi*
Biomedical Research on Trace Elements, 28(1), p.1 - 10, 2017/04
Radionuclides are commonly determined with radiometry and mass spectrometry. For -emitting nuclides, the activities can be measured without chemical separation due to the strong penetration ability. In contrast, the measurements of alpha and beta-emitting nuclides are generally associated with tedious and time-consuming chemical separation procedures to remove concomitants. Thus, an adsorbent that achieves rapid separation is desirable to reduce separation time and workload. Our research team has developed compact cartridge-type solid phase extraction materials which enable to facilitate separation procedures. In this review, basic separation performances of the developed cartridges were overviewed along with two application examples to radionuclide-containing samples.
Takagai, Yoshitaka*; Furukawa, Makoto*; Kameo, Yutaka; Matsueda, Makoto; Suzuki, Katsuhiko*
Bunseki Kagaku, 66(4), p.223 - 231, 2017/04
no abstracts in English
Esaka, Fumitaka; Yasuda, Kenichiro; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki
Talanta, 165, p.122 - 127, 2017/04
The isotope ratios of Pu/Pu, Pu/Pu, Pu/Pu, and Pu/Pu were measured for individual Pu and U-Pu mixed oxide particles by a combination of alpha spectrometry and inductively coupled plasma mass spectrometry (ICP-MS). As a consequence, we were able to determine the Pu/Pu, Pu/Pu, and Pu/Pu isotope ratios with ICP-MS after particle dissolution and chemical separation of uranium, plutonium and americium with UTEVA resins. Furthermore, Pu/Pu isotope ratios were able to be calculated by using both the Pu/( Pu+Pu) activity ratios that had been measured through alpha spectrometry and the Pu/Pu isotope ratios determined through ICP-MS. Therefore, the combined use of alpha spectrometry and ICP-MS is useful in determining plutonium isotope ratios, including Pu/Pu, in individual U-Pu mixed oxide particles.
Konda, Miki; Asai, Shiho; Hanzawa, Yukiko; Magara, Masaaki
JAEA-Technology 2015-054, 22 Pages, 2016/03
Isotope dilution mass spectrometry (IDMS) with ICP-MS is reliable method for determination of Zr-93, which is one of the long-lived fission products found in spent nuclear fuel and high-level radioactive wastes. In order to use an isotope standard solution of zirconium as the spike for IDMS, dissolving a commercially available solid isotope standard is indispensable. Prior to the dissolution of the Zr-91 isotope standard, solubility of metal zirconium in a mixture of HNO and HF was evaluated using zirconium metal chips. Then, 2 mg of the Zr-91 isotope standard was dissolved with 0.2 mL of 1 M HNO-3 v/v% HF mixed solution, followed by adjusting the concentration of Zr-91 to approximately 1,000 g/g. IDMS, in which a natural isotopic abundance standard solution of zirconium was used as the spike, was employed for the determination of the concentration of Zr-91 in the prepared Zr-91 isotope standard solution. The concentration of Zr-91 in the prepared Zr-91 isotope standard solution was (9.61.0) 10 g/g, which is in good agreement with the predicted concentration. This indicates that the Zr-91 metal isotope standard was completely dissolved with sufficient chemical stability. Additionally, no impurities were detected in the prepared Zr-91 isotope standard solution. These positive results denote that the Zr-91 isotope standard solution with the preferable quality for IDMS of Zr-93 can be obtained by the proposed dissolution procedures.
Asai, Shiho; Hanzawa, Yukiko; Konda, Miki; Suzuki, Daisuke; Magara, Masaaki; Kimura, Takaumi; Ishihara, Ryo*; Saito, Kyoichi*; Yamada, Shinsuke*; Hirota, Hideyuki*
Analytical Chemistry, 88(6), p.3149 - 3155, 2016/03
Neptunium-237 (Np) is one of the major long-lived radionuclides found in spent nuclear fuel. To evaluate the long-term safety of a HLW repository, the Np content in spent nuclear fuel must be determined. In this study, micro-volume anion-exchange porous polymer disk-packed cartridges were prepared for Am-Np separation, which is required prior to the measurement of Np with ICP-MS. Disks with a volume of 0.08 cm were cut out from porous sheets having triethylenediamine (TEDA)-containing polymer chains densely attached on the pore surface. The resulting TEDA-introduced disk cartridge was applied to a spent nuclear fuel sample. The chemical yield of Np was 90.4%, which is sufficiently high for ICP-MS measurement of Np. Compared with the conventional separation technique using commercially available anion-exchange resin columns, the time required to adsorb, wash and elute Np using the TEDA-introduced disk cartridge was reduced by 75%.
Esaka, Fumitaka; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki
Journal of Radioanalytical and Nuclear Chemistry, 306(2), p.393 - 399, 2015/11
An analytical technique was developed by a combination of single particle dissolution, chemical separation of uranium, plutonium and americium with extraction chromatography using UTEVA resins and measurement with inductively coupled plasma mass spectrometry (ICP-MS). This method was applied to plutonium isotope ratio analysis of individual U-Pu particles with U/Pu ratios ranging from 1 to 70. Consequently, Pu/Pu, Pu/Pu and Pu/Pu isotope ratios were successfully determined, while it was impossible to determine Pu/Pu ratios due to the high process blank values on m/z 238.
Asai, Shiho; Limbeck, A.*
Talanta, 135, p.41 - 49, 2015/04
A new analytical method for chondrite-normalized Rare earth elements (REE) plot has been developed in this study. Cation-exchange resin particles were used as a substrate to retain REE for laser ablation inductively coupled plasma mass spectrometry (LA-ICP-MS). In LA analysis, formation of oxide and hydroxide of the light REE and Ba which causes spectral interferences in the heavy REE measurement was effectively attenuated, compared to conventional solution nebulization ICP-MS. To evaluate the applicability of the proposed method, the REE-adsorbed particles prepared by immersing them in a U-bearing solution were measured with LA-ICP-MS. Additionally, each concentration of REE in the U standard solution was determined with solution nebulization ICP-MS. The chondrite-normalized plot obtained through LA-ICP-MS analysis exhibited close agreement with that obtained through the solution nebulization ICP-MS of the REE-separated solution within the uncertainties.
Kokubu, Yoko; Yasuda, Kenichiro; Magara, Masaaki; Miyamoto, Yutaka; Sakurai, Satoshi; Usuda, Shigekazu; Yamazaki, Hideo*; Yoshikawa, Shusaku*
Journal of Radioanalytical and Nuclear Chemistry, 273(1), p.183 - 186, 2007/07
no abstracts in English
Chai, J.; Miyamoto, Yutaka; Kokubu, Yoko; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu; Oura, Yasuji*; Ebihara, Mitsuru*
Journal of Radioanalytical and Nuclear Chemistry, 272(2), p.397 - 401, 2007/05
Cm is an important nuclide because it has the next-shortest half-life (1.610 yr) from Pu among the transuranic nuclides. The disintegration of Cm to U by three decays and two decays and the chemical fractionation between Cm and U during the formation of solid materials in early solar system lead to changes in the ratios of U to U. This variation may provide strict constraints on the time interval between the last r-process nucleosynthetic event and the formation of the solar system. It is important to develop a practical analysis protocol to determine the isotope ratio of trace uranium in geochemical and environment samples. As uranium is the least abundant element in our solar system, analytical techniques with high sensitivity and precision are required. In this study, a double focusing inductively coupled plasma mass spectory was applied to measure isotopic ratio of uranium. By one set data obtained from the EDTA phase of the Jilin meteorite sample, the upper limit of Cm in the early solar system was calculated and Cm/U 0.003 was obtained.
Kokubu, Yoko; Yasuda, Kenichiro; Magara, Masaaki; Miyamoto, Yutaka; Sakurai, Satoshi; Usuda, Shigekazu; Yamazaki, Hideo*; Mitamura, Muneki*; Yoshikawa, Shusaku*
Journal of Geosciences, Osaka City University, 50, p.7 - 13, 2007/03
no abstracts in English
Magara, Masaaki; Usuda, Shigekazu; Sakurai, Satoshi; Watanabe, Kazuo; Esaka, Fumitaka; Hirayama, Fumio; Lee, C. G.; Yasuda, Kenichiro; Kono, Nobuaki; Inagawa, Jun; et al.
Dai-26-Kai Kaku Busshitsu Kanri Gakkai (INMM) Nippon Shibu Nenji Taikai Rombunshu, p.157 - 164, 2005/00
JAERI has conducted the analysis of domestic and the IAEA samples. JAERI is developing the analytical techniques to improve the analytical ability for the safeguards environmental samples. For bulk analysis, study is focused on the improvement of reliability of isotope ratio measurements by ICP-MS. New chemical separation techniques are under development and a desolvation module is introduced to reduce the polyatomic interferences. In particle analysis, the sample preparation procedure for SIMS method is modified to measure the U/U and U/U ratios for individual particles. We are also developing fission track-TIMS method to measure uranium isotope ratios in particles of sub-micrometer size. A screening instrument of X-ray fluorescent analysis is equipped to measure elemental distribution on a swipe surface.
Fu, F.; Akagi, Tasuku*; Suzuki, Yuichiro*; Watanabe, Kazuo; Yabuki, Sadayo*
Geochemical Journal, 38(4), p.333 - 343, 2004/08
no abstracts in English