The Laboratory Operation Based on ISO/IEC 17025; Radioactivity analysis of environmental samples by germanium semiconductor detectors

Urushidate, Tadayuki*; Yoda, Tomoyuki; Otani, Shuichi*; Yamaguchi, Toshio*; Kunii, Nobuaki*; Kuriki, Kazuki*; Fujiwara, Kenso; Niizato, Tadafumi; Kitamura, Akihiro; Iijima, Kazuki

JAEA-Review 2022-023, 8 Pages, 2022/09

JAEA-Review-2022-023.pdf:1.19MB

After the accident of the Fukushima Daiichi Nuclear Power Station, the Japan Atomic Energy Agency has newly set up a laboratory in Fukushima and started measuring radioactivity concentrations of environmental samples. In October 2015, Fukushima Radiation Measurement Group has been accredited the ISO/IEC 17025 standard by the Japan Accreditation Board (JAB) as a testing laboratory for radioactivity analysis (Cs, Cs) based on Gamma-ray spectrometry with germanium semiconductor detectors. The laboratory has measured approximately 60,000 of various environmental samples at the end of March 2022. The laboratory quality control and measurement techniques have been accredited by regular surveillance of JAB. In September 2019, the laboratory renewed accreditation as a testing laboratory for radioactivity analysis.

Developing accelerator mass spectrometry capabilities for anthropogenic radionuclide analysis to extend the set of oceanographic tracers

Hain, K.*; Martschini, M.*; Glce, F.*; Honda, Maki; Lachner, J.*; Kern, M.*; Pitters, J.*; Quinto, F.*; Sakaguchi, Aya*; Steier, P.*; et al.

Frontiers in Marine Science (Internet), 9, p.837515_1 - 837515_17, 2022/03

https://doi.org/10.3389/fmars.2022.837515

Recent major advances in accelerator mass spectrometry (AMS) at the Vienna Environmental Research Accelerator (VERA) regarding detection efficiency and isobar suppression have opened possibilities for the analysis of additional long-lived radionuclides at ultra-low environmental concentrations. These radionuclides, including U, Cs, Tc and Sr, will become important for oceanographic tracer application due to their generally conservative behavior in ocean water. In particular, the isotope ratios U/U and Cs/Cs have proven to be powerful fingerprints for emission source identification as they are not affected by elemental fractionation. Improved detection efficiencies allowed us to analyze all major long-lived actinides, i.e. U, Np, Pu, Am as well as the very rare U, in the same 10 L water samples of an exemplary depth profile from the northwest Pacific Ocean. Especially for Sr analysis, our new approach has already been validated for selected reference materials (e.g. IAEA-A-12) and is ready for application in oceanographic studies. We estimate that a sample volume of only (1-3) L ocean water is sufficient for Sr as well as Cs analysis, respectively.

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.

A Cubic CeBr gamma-ray spectrometer suitable for the decommissioning of the Fukushima Daiichi Nuclear Power Station

Kaburagi, Masaaki; Shimazoe, Kenji*; Otaka, Yutaka*; Uenomachi, Mizuki*; Kamada, Kei*; Kim, K. J.*; Yoshino, Masao*; Shoji, Yasuhiro*; Yoshikawa, Akira*; Takahashi, Hiroyuki*; et al.

Nuclear Instruments and Methods in Physics Research A, 971, p.164118_1 - 164118_8, 2020/08

https://doi.org/10.1016/j.nima.2020.164118

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.

Guidance for gamma spectrometry intercomparison based on the information obtained through five intercomparisons during the Fukushima mapping project

Mikami, Satoshi; Ishikawa, Daisuke*; Matsuda, Hideo*; Hoshide, Yoshifumi*; Okuda, Naotoshi*; Sakamoto, Ryuichi*; Saito, Kimiaki

Journal of Environmental Radioactivity, 210, p.105938_1 - 105938_7, 2019/12

https://doi.org/10.1016/j.jenvrad.2019.03.014

Five intercomparisons of in situ spectrometry by 6-7 participating teams have been conducted between December 2011 and August 2015 at sites in Fukushima prefecture which affected by the fallout of FDNPS accident occurred in March 2011. The evaluated deposition densities agreed within 5-6% in terms of coefficient of variation (CV) for radiocesium (Cs and Cs), by our best achievement, and the ratio of Cs/Cs in deposition density agreed within 1-2% in CV, through five intercomparisons. These results guarantee the accuracy of the measurements of the mapping project. Two different methods for intercomparison were conducted: (1) sequential measurements at an identical point; and (2) simultaneous measurements in a narrow area within 3 m radius. In a comparison between the two methods at a site, no significant difference was observed between the results. The standard protocols for the two different intercomparison methods were proposed based on our experience.

Measurements of thermal-neutron capture cross-section and resonance integral of neptunium-237

Nakamura, Shoji; Kitatani, Fumito; Kimura, Atsushi; Uehara, Akihiro*; Fujii, Toshiyuki*

Journal of Nuclear Science and Technology, 56(6), p.493 - 502, 2019/06

https://doi.org/10.1080/00223131.2019.1598304

The thermal-neutron capture cross-section()and resonance integral(I) were measured for the Np(n,)Np reaction by an activation method. A method with a Gadolinium filter, which is similar to the Cadmium difference method, was used to measure the with paying attention to the first resonance at 0.489 eV of Np, and a value of 0.133 eV was taken as a cut-off energy. Neptunium-237 samples were irradiated at the pneumatic tube of the Kyoto University Research Reactor in Institute for Integral Radiation and Nuclear Science, Kyoto University. Wires of Co/Al and Au/Al alloys were used as monitors to determine thermal-neutron fluxes and epi-thermal Westcott's indices at an irradiation position. A -ray spectroscopy was used to measure activities of Np, Np and neutron monitors. On the basis of Westcott's convention, the and I values were derived as 186.96.2 barn, and 100990 barn, respectively.

Ion desorption from bulk cesium chloride at moderate temperature (500C) under electric field

Baba, Yuji; Shimoyama, Iwao

e-Journal of Surface Science and Nanotechnology (Internet), 16, p.53 - 59, 2018/03

https://doi.org/10.1380/ejssnt.2018.53

Surface ionization for cesium chloride and Cs-adsorbed soil has been investigated. For cesium chloride, neutral cesium was desorbed around 645C which is close to the melting point of cesium. While Cs ion was desorbed from 400C. The ratio of desorbed ions and neutrals (Cs/Cs) has a maximum around 410 C. Temperature dependence of Cs/Cs was analyzed using Saha-Langmuir equation, As a result, it was found that the temperature maximum is due to the changes of the surface work function induced by the phase transition of CsCl.

High precision analysis of isotopic composition for samples used for nuclear cross-section measurements

Shibahara, Yuji*; Hori, Junichi*; Takamiya, Koichi*; Fujii, Toshiyuki*; Fukutani, Satoshi*; Sano, Tadafumi*; Harada, Hideo

EPJ Web of Conferences, 146, p.03028_1 - 03028_4, 2017/09

https://doi.org/10.1051/epjconf/201714603028

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.