Source term identification of environmental radioactive Pu/U particles by their characterization with non-destructive spectrochemical analytical techniques |
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Institution: | 1. Institut für Nukleare Entsorgung, Karlsruhe Institute of Technology, P.O. Box 3640, D-76021 Karlsruhe, Germany;2. Institute for Nuclear Chemistry, University of Mainz, 55099 Mainz, Germany |
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Abstract: | Six radioactive particles stemming from Thule area (NW-Greenland) were investigated by gamma-ray and L X-ray spectrometry based on radioactive disintegration, scanning electron microscopy coupled with energy-dispersive and wavelength-dispersive X-ray spectrometer, synchrotron radiation based techniques as microscopic X-ray fluorescence, microscopic X-ray absorption near-edge structure (μ-XANES) as well as combined X-ray absorption and fluorescence microtomography. Additionally, one particle from Mururoa atoll was examined by microtomography. From the results obtained, it was found out that the U and Pu were mixed in the particles. The U/Pu intensity ratios in the Thule particles varied between 0.05 and 0.36. The results from the microtomography showed that U/Pu ratio was not homogeneously distributed. The 241Am/238 + 239 + 240Pu activity ratios varied between 0.13 and 0.17, indicating that the particles originate from different source terms. The oxidation states of U and Pu as determined by μ-XANES showed that U(IV) is the preponderant species and for Pu, two types of particles could be evidenced. One set had about 90% Pu(IV) while in the other the ratio Pu(IV)/Pu(VI) was about one third. |
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