Stable hydrogen and oxygen isotope analyses of geological samples using a thermal conversion elemental analyzer-isotope ratio mass spectrometer at Tono Geoscience Center

Yamamoto, Yusuke*; Watanabe, Takahiro; Niwa, Masakazu; Shimada, Koji

JAEA-Testing 2023-003, 67 Pages, 2024/02

JAEA-Testing-2023-003.pdf:4.63MB

A long-term geosphere stability for geological disposal is evaluated by the past geological environmental changes and modern conditions. Stable hydrogen and oxygen isotope ratios (D, O) of geological samples are useful information to estimate the past environmental changes and modern conditions. Recently, the thermal conversion elemental analyzer and isotope ratio mass spectrometer (TC-EA/IRMS) were installed in the Tono Geoscience Center for D and O measurements of geological samples. In this study, we reported analytical methods of D and O using international standard reference materials. In addition, evaluation tests of uncertainty by repeated analyses of the standards were performed using the TC-EA/IRMS. Furthermore, the D and O analyses by the TC- EA/IRMS were also applied to fault rock samples.

Determination of Cs/Cs isotopic ratio in soil collected near Fukushima Daiichi Nuclear Power Station through mass spectrometry

Shimada, Asako; Tsukahara, Takehiko*; Nomura, Masao*; Kim, M. S.*; Shimada, Taro; Takeda, Seiji; Yamaguchi, Tetsuji

Journal of Nuclear Science and Technology, 58(11), p.1184 - 1194, 2021/11

https://doi.org/10.1080/00223131.2021.1931520

Determining the completeness of nuclear reactor decommissioning is an important step in safely utilizing nuclear power. For example, Cs from the Fukushima Daiichi Nuclear Power Station (FDNPS) accident can be treated as background radioactivity, so determining the origin of Cs is essential. To accomplish this, measuring the Cs/Cs isotope ratio can be useful, so this study optimized a solvent extraction method, with calix[4]arene-bis(t-octylbenzo-crown-6) [BOBCalixC6] in 1-octanol, to purify radioactive Cs, radiocesium, from a solution of major environmental soil elements and mass spectrometry interference elements. This optimized method was applied to Cs purification in soil samples (40 g), and the final solutions contained a total of 10g/ml of the major soil elements and ng/ml concentrations at most of interfering elements. Soil samples collected near the FDNPS were then purified, and the Cs/Cs isotope ratios were measured, using both thermal ionization mass spectrometry (TIMS) and triple quadrupole induced coupled plasma mass spectrometry (ICP-QQQ). The results of each of these measurements were compared, and we found that Cs isotope ratios obtained by TIMS were more precise, by an order of magnitude, while the ICP-QQQ results possessed good abundance sensitivities. A slightly higher Cs/Cs ratio in the northwest area of the FDNPS was observed, while other areas exhibited similar values, all within the measurement error range, which indicated different origins of radiocesium. These results agreed with previously reported Cs/Cs activity distributions, suggesting that this ratio may be useful in identifying radiocesium origins for evaluating future nuclear reactor decommissions.

Effect of surface conditions of the filament used in thermal ionization mass spectrometry on an uranium isotopic measurement

Taguchi, Shigeo; Miyauchi, Hironari*; Horigome, Kazushi; Yamamoto, Masahiko; Kuno, Takehiko

Bunseki Kagaku, 67(11), p.681 - 686, 2018/11

https://doi.org/10.2116/bunsekikagaku.67.681

In thermal ionization mass spectrometry, de-gassing is one of the important treatments to release impurities of filaments and to minimize the influence of background. In this work, the effect of the surface change in the tungsten filament induced by the conductively heating treatment on uranium isotopic (U/U) measurement has been investigated. It was found that the conductively heating treatment of the filament has the effect of smoothing the surface of the filament and also has the effect of improving the deposition of the sample on the filament surface. As a result of either these effects, the precision of uranium isotopic (U/U) measurement was improved.

Determination of plutonium isotope ratios in individual uranium-plutonium mixed particles with inductively coupled plasma mass spectrometry

Esaka, Fumitaka; Suzuki, Daisuke; Miyamoto, Yutaka; Magara, Masaaki

Journal of Radioanalytical and Nuclear Chemistry, 306(2), p.393 - 399, 2015/11

https://doi.org/10.1007/s10967-015-4113-6

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.

Distribution of plutonium isotopes and Cs found in the surface soils of Nagasaki, Japan

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

Report for 46th INMM annual meeting and visit to nuclear research institutes in USA

Magara, Masaaki

Kaku Busshitsu Kanri Senta Nyusu, 34(11), P. 18, 2005/11

no abstracts in English

Efficient isotope ratio analysis of uranium particles in swipe samples by total-reflection X-ray fluorescence spectrometry and secondary ion mass spectrometry

Esaka, Fumitaka; Watanabe, Kazuo; Fukuyama, Hiroyasu; Onodera, Takashi; Esaka, Konomi; Magara, Masaaki; Sakurai, Satoshi; Usuda, Shigekazu

Journal of Nuclear Science and Technology, 41(11), p.1027 - 1032, 2004/11

https://doi.org/10.3327/jnst.41.1027

A new particle recovery method and a sensitive screening method were developed for subsequent isotope ratio analysis of uranium particles in safeguards swipe samples. The particles in the swipe sample were recovered onto a carrier by means of vacuum suction 8211; impact collection method. When grease coating was applied to the carrier, the recovery efficiency was improved to 48 %, which is superior to that of conventionally-used ultrasoneration method. Prior to isotope ratio analysis with secondary ion mass spectrometry (SIMS), total reflection X-ray fluorescence spectrometry (TXRF) was applied to screen the sample for the presence of uranium particles. By the use of Si carriers in TXRF analysis, the detection limit of 22 pg was achieved for uranium. By combining these methods with SIMS, the isotope ratios of U/U for individual uranium particles were efficiently determined.

Isotope ratio analysis of individual particles containing nuclear materials in safeguards environmental samples

Esaka, Fumitaka

Bunseki, 2003(11), p.688 - 691, 2003/11

https://ci.nii.ac.jp/naid/10012533226

Isotope ratio measurement for individual particles containing uranium in swipe samples taken at nuclear facilities is a powerful tool to verify the absence of undeclared nuclear activities. In order to develop the analysis technique, we have investigated a series of methods: particle recovery from the swipe sample, particle screening and isotope ratio analysis for individual particles. As the result, the 235U/238U ratio was determined with the relative standard deviation within 2.0 % for the particle with a diameter of 1 um.

Development for ultra-trace analysis method of U and Pu in safeguards environmental samples at the clean facility

Takahashi, Masato; Magara, Masaaki; Sakurai, Satoshi; Kurosawa, Setsumi; Esaka, Fumitaka; Taguchi, Takuji; Takai, Konomi; Fukuyama, Hiroyasu; Lee, C. G.; Yasuda, Kenichiro; et al.

Dai-23-Kai Kaku Busshitsu Kanri Gakkai Nihon Shibu Nenji Taikai Rombunshu, 8 Pages, 2002/09

Based on the strengthen safeguard program of the IAEA to detect undeclared nuclear activities, the method of precise and accurate isotope ratio determination for uranium and plutonium in the environmental samples (cotton swipes) has been developed at JAERI. The samples should be treated in clean environment in order to secure the analytical reliability by eliminating external contamination from the samples containing trace amount of uranium and plutonium. Since the measurement by ICP-MS is favorable to bulk analysis from view points of analytical capacity and operation simplicity, we have studied sample preparation procedures for the trace amount of uranium and plutonium to be applied to ICP-MS. Up to the present, interfering factors involved during analytical processes and the ICP-MS measurement of uranium and plutonium were examined. As a result, uranium and plutonium isotope measurement more than 100 pg and 100 fg, respectively, became possible at JAERI clean facility. At presentation, other progress in the development will be reported.

JAERI Clean Laboratory for Environmental Analysis and Research; Its specific feature and R&D program

Sakurai, Satoshi; Hanzawa, Yukiko; Magara, Masaaki; Usuda, Shigekazu; Watanabe, Kazuo; Adachi, Takeo

Kuki Seijo, 39(6), p.404 - 410, 2002/03

https://ci.nii.ac.jp/naid/10007973949

no abstracts in English