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Uranium-Containing Glassy Aerosol Microparticles Emitted during Fukushima Daiichi Nuclear Accident Reached Tsukuba -Multiple X-ray analyses using synchrotron radiation X-ray microbeam- (Press Release)

Release Date
08 Aug, 2014
  • BL37XU (Trace Element Analysis)

Tokyo University of Science

A research group led by Izumi Nakai (professor) and Yoshinari Abe (assistant professor) of Tokyo University of Science (Chairman of the Board of Directors, Shigeru Nakane) conducted joint research with Yasuhito Igarashi and Kouji Adachi of the Meteorological Research Institute and Yasuko Terada of the Japan Synchrotron Radiation Research Institute (JASRI) for the purpose of clarifying the properties of radioactive materials emitted during the Fukushima Daiichi Nuclear Power Plant (FDNPP) accident. They carried out multiple X-ray analyses at SPring-8 for radioactive aerosol microparticles [called cesium (Cs) balls] collected at the Meteorological Research Institute in Tsukuba City immediately after the accident. As a result, they found that the Cs balls contained not only Cs but also uranium (U) and its fission products and that the Cs balls were present in the glassy state with a high oxidation state. These results provide chemical evidence that the fuel rods melted and fell to the bottom of the containment vessel during the accident. The achievements of this study were published in the American Chemical Society (ACS) journal Analytical Chemistry.

Publication:
"Detection of Uranium and Chemical State Analysis of Individual Radioactive Microparticles Emitted from the Fukushima Nuclear Accident Using Multiple Synchrotron Radiation X‑ray Analyses"
Y. Abe, Y. Iizawa, Y. Terada, K. Adachi, Y. Igarashi, I. Nakai
Analytical Chemistry
DOI:10.1021/ac501998d

Details of study
   Cs balls are spherical particles with a diameter of approximately 2 µm and contain radioactive Cs, as indicated by their name. It has been pointed out that Cs balls were emitted during the FDNPP accident. The research group carried out X-ray analyses of Cs balls using BL37XU X-rays focused to a width and height of 1 µm or smaller for examining the chemical composition, chemical state, and crystal structure of the Cs balls at the single-particle level nondestructively and in detail.
   First, X-ray fluorescence analysis was performed using a high-energy X-ray (37.5 keV) to identify the elements other than Cs in the Cs balls. The results indicated that the elements considered to be the fission products of U fuel, such as barium (Ba), rubidium (Rb), and molybdenum (Mo), were contained in the Cs balls. In addition, U fuel itself was also detected in some Cs balls (Fig.1). These results suggest that not only was highly volatile Cs emitted from the FDNPP into the atmosphere but also the plant was damaged sufficiently to emit the U fuel to the outside.
   Moreover, elements originating from the components of the plant structure, such as silicon (Si), iron (Fe), and zinc (Zn), were also detected in the Cs balls. X-ray absorption near-edge structure and X-ray diffraction analyses revealed that the Cs balls were formed in the high-oxidation glassy states (Fe3+, Mo6+, Sn4+). These results indicate a scenario in which the fuel, containment vessel, and plant structures were melted and mixed in the plant during the accident and the mixture was emitted into the atmosphere and rapidly cooled to form Cs balls in the glassy state. This scenario gives chemical support to the hypothesis that the fuel rods melted and fell to the bottom of the containment vessel during the accident.
   Thus far, the possibility that U emitted during the accident reached near the Kanto Region has been already pointed out. However, how the heavy material U was dispersed in the environment has remained unclear. The research group clarified that the glass microparticles were one of the carriers of U.
   As above, nondestructive X-ray analyses of particles with a diameter of only 2 µm provided much information on the state of the plant during the accident and the emission of radioactive materials into the atmosphere. This could be only realized by multiple X-ray analyses using a SPring-8 synchrotron radiation X-ray microbeam. The achievements of this study were published in the ACS journal Analytical Chemistry.


《Figures》

図1.micro-XRF imaging
Fig.1  Distributions of U, Cs, and Ba in Cs ball (lower right, SEM image)




図2.micro-XANES analysis
Fig.2  X-ray absorption spectrum clearly showing the presence of U




For more information, please contact:

    Prof. Izumi Nakai (Tokyo University of Science )
    E-mail:mail1

    Assistant Prof. Yoshinari Abe (Tokyo University of Science )
    E-mail:mail2

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