Novel Sr analysis of environmental samples by ion-laser interaction mass spectrometry

Honda, Maki; Martschini, M.*; Marchhart, O.*; Priller, A.*; Steier, P.*; Golser, R.*; Sato, Tetsuya; Tsukada, Kazuaki; Sakaguchi, Aya*

Analytical Methods, 14(28), p.2732 - 2738, 2022/07

https://doi.org/10.1039/D2AY00604A

The sensitive Sr analysis with accelerator mass spectrometry (AMS) was developed for the advances of environmental radiology. One advantage of AMS is the ability to analyze various environmental samples with Sr/Sr atomic ratios of 10 in a simple chemical separation. Three different IAEA samples with known Sr concentrations (moss-soil, animal bone, Syrian soil: 1 g each) were analyzed to assess the validity of the chemical separation and the AMS measurement. The Sr measurements were conducted on the AMS system combined with the Ion Laser InterAction MasSpectrometry (ILIAMS) setup at the University of Vienna, which has excellent isobaric separation performance. The isobaric interference of Zr in the Sr AMS was first removed by chemical separation. The separation factor of Zr in two-step column chromatography with Sr resin and anion exchange resin was 10. The Zr remaining in the sample was removed by ILIAMS effectively. This simple chemical separation achieved a limit of detection 0.1 mBq in the Sr AMS, which is lower than typical -ray detection. The agreement between AMS measurements and nominal values for the Sr concentrations of IAEA samples indicated that the new highly-sensitive Sr analysis in the environmental samples with AMS is reliable even for high matrix samples of soil and bone.

Incorporation of U, Pb and rare earth elements in calcite through crystallisation from amorphous calcium carbonate; Simple preparation of reference materials for microanalysis

Miyajima, Yusuke*; Saito, Ayaka*; Kagi, Hiroyuki*; Yokoyama, Tatsunori; Takahashi, Yoshio*; Hirata, Takafumi*

Geostandards and Geoanalytical Research, 45(1), p.189 - 205, 2021/03

https://doi.org/10.1111/ggr.12367

Uncertainty for elemental and isotopic analyses of calcite by LA-ICP-MS is largely controlled by the homogeneity of the reference materials (RMs) used for normalization and validation. In order to produce calcite RMs with homogeneous elemental and isotopic compositions, we incorporated elements including U, Pb, and rare earth elements into calcite through heat- and pressure-induced crystallization from amorphous calcium carbonate that was precipitated from element-doped reagent solution. X-ray absorption spectra showed that U was present as U(VI) in the synthesized calcite, probably with a different local structure from that of aqueous uranyl ions. The uptake rate of U by our calcite was higher in comparison to synthetic calcite of previous studies. Variations of element mass fractions in the calcite were better than 12% 2RSD, mostly within 7%. The Pb/Pb ratio in the calcite showed 1% variations, while the U/Pb ratio showed 3-24% variations depending on element mass fractions. Using the synthetic calcite as primary RMs, we could date a natural calcite RM, WC-1, with analytical uncertainty as low as 3%. The method presented can be useful to produce calcite with controlled and homogeneous element mass fractions, and is a promising alternative to natural calcite RMs for U-Pb geochronology.

Vertical distributions of Iodine-129 and iodide in the Chukchi Sea and Bering Sea

Miwa, Kazuji; Obata, Hajime*; Suzuki, Takashi

Journal of Nuclear Science and Technology, 57(5), p.537 - 545, 2020/05

https://doi.org/10.1080/00223131.2019.1699189

This study investigated the vertical distribution of Iodine-129 (I) which is mainly produced by European nuclear reprocessing plants in the Chukchi Sea and Bering Sea. I was found to be distributed almost uniformly in fallout level, and an increasing in I concentration levels caused by high I water inflow from the Atlantic Ocean was not observed. Additionally, we revealed the vertical distribution of iodide, one chemical form of iodine, from the Bering Shelf area to the Chukchi Sea for the first time. The increasing tendency of iodide near sea bottom was observed.

Activation measurement for thermal-neutron capture cross-section of Cesium-135

Nakamura, Shoji; Kimura, Atsushi; Iwamoto, Osamu; Shibahara, Yuji*; Uehara, Akihiro*; Fujii, Toshiyuki*

KURNS Progress Report 2018, P. 106, 2019/08

https://www.rri.kyoto-u.ac.jp/PUB/report/PR/ProgRep2018/ProgRep2018.html

Under the ImPACT project, the neutron capture cross-section measurements of Cesium-135 (Cs) among the long-lived fission products have been performed at Kyoto University. This paper reports measurements of the thermal-neutron capture cross-section of Cs at the Kyoto University Research Reactor (KUR).

Inductively coupled plasma-mass spectrometry

Esaka, Fumitaka

Analytical Sciences, 33(10), p.1097 - 1098, 2017/10

https://doi.org/10.2116/analsci.33.1097

Inductively coupled plasma-mass spectrometry (ICP-MS) is widely used in various fields such as environmental, geological, and clinical sciences. In this report, recent advances of the ICP-MS analysis and expected applications are described.

Application of automated particle screening for effective analysis of individual uranium particles by thermal ionization mass spectrometry

Esaka, Fumitaka; Suzuki, Daisuke; Yomogida, Takumi; Magara, Masaaki

Analytical Methods, 8(7), p.1543 - 1548, 2016/02

AA2015-0572.pdf:0.66MB

https://doi.org/10.1039/C5AY02841H

The isotope ratio analysis of individual uranium particles in environmental samples taken at nuclear facilities is important to clarify their origins for nuclear safeguards. In the present study, automated particle screening was used to select uranium particles prior to precise isotope ratio analysis by thermal ionization mass spectrometry (TIMS). As a result, molecular ion interferences on the uranium mass region were able to be almost completely avoided in the analysis of real inspection samples using APM-TIMS. Therefore, the performance of APM-TIMS was sufficient for obtaining isotope ratio data of individual particles without molecular ion interferences.

Mass-spectrometric study of PuCd

Nakajima, Kunihisa; Arai, Yasuo; Yamashita, Toshiyuki

Journal of Physics and Chemistry of Solids, 66(2-4), p.639 - 642, 2005/02

https://doi.org/10.1016/j.jpcs.2004.06.072

PuCd intermetallic compound was prepared by heating pure Pu and Cd metals at about 950K. PuCd was found to be a prototype of CdI by means of powder X-ray diffractometry. Mass-spectrometric experiment was performed in the temperature range of 650-770K. It was found that the vapor pressures of Cd over PuCd+Pu were three to five orders of magnitude lower than those over Cd in this temperature range. From these vapor pressures, Gibbs free energy of formation of PuCd was evaluated.

Development of frequency stabilized laser system for long-lived isotope analysis, 1; Development of Littrow configuration extended cavity diode laser

Miyabe, Masabumi; Oda, Koichi*; Oba, Masaki; Kato, Masaaki; Wakaida, Ikuo; Watanabe, Kazuo

JAERI-Tech 2004-064, 33 Pages, 2004/10

JAERI-Tech-2004-064.pdf:1.89MB

In nuclear waste materials there are various radionuclides to which standard analytical techniques are difficult to be applied. We are developing an analytical technique where such nuclides are analyzed using multi-step resonance ionization mass spectrometry. In this study, we have developed an external cavity diode laser applicable to the analysis. The wavelength and output power dependence on injection current and temperature were investigated for various types of laser diodes. Based on the data, we have obtained a suitable condition to operate the ECDL in stable single-mode oscillation, so that a continuous scanning range of about 100 GHz was realized. Additionaly, to evaluate the bandwidth of the developed ECDL, we have performed Doppler-free spectroscopy. The reasonable agreement of the measured isotope shift and HFS splitting with the reported values demonstrated that the developed ECDL is applicable to a precise laser spectroscopy as well as a laser trace analysis.

Coexistence of passive and active oxidation for O/Si(001) system observed by SiO mass spectrometry and synchrotron radiation photoemission spectroscopy

Teraoka, Yuden; Moritani, Kosuke; Yoshigoe, Akitaka

Applied Surface Science, 216(1-4), p.8 - 14, 2003/06

https://doi.org/10.1016/S0169-4332(03)00479-3

The experiments concerning the oxidation of Si(001) were performed at the surface reaction analysis apparatus, installed at the beamline BL23SU in the SPring-8. The SiO desorb remarkably at surface temperature of 1000 K. The desorption yield increased with increasing the incident energy of O. On the other hand, the desorption yield increased with decreasing the incident energy in the temperature region lower than 1000 K. Oxygen uptake curves observed by O-1s photoemission measurements corresponded to the SiO desorption features. These facts reveal that the passive oxidation coexists with the SiO desorption in the temperature region from 900 K to 1000 K.

Mass-spectrometric determination of oxygen potential of hypostoichiometric urania-yttria solid solution

Nakajima, Kunihisa; Omichi, Toshihiko*; Arai, Yasuo

Journal of Nuclear Materials, 304(2-3), p.176 - 181, 2002/08

https://doi.org/10.1016/S0022-3115(02)00876-0

The oxygen potentials of two type urania-yttria solid solutions, one is the solid solution expressed as nearly UYO and the other is nearly stoichiometric solid solution, are investigated by use of a mass spectrometer combined with a Knudsen cell. The oxygen potentials for the nearly stoichiometric specimens are much higher than those for pure urania with similar stoichiometry. On the other hand, the oxygen potentials for fully reduced specimens almost agree with those for pure urania having the same oxygen deficiencis.