Spatially resolved analysis of plutonium isotopic signatures in environmental particle samples by laser ablation-MC-ICP-MS

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• 作者：Stefanie Konegger-Kappel ; Thomas Prohaska
• 关键词：Plutonium isotope ratios ; Environmental contamination ; Chernobyl nuclear power plant ; (MC) ; ICP ; MS ; Laser ablation
• 刊名：Analytical and Bioanalytical Chemistry
• 出版年：2016
• 出版时间：January 2016
• 年：2016
• 卷：408
• 期：2
• 页码：431-440
• 全文大小：3,506 KB
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• 作者单位：Stefanie Konegger-Kappel (1) (2)
  Thomas Prohaska (1)
  
  1. Department of Chemistry, Division of Analytical Chemistry, Research Group Analytical Ecogeochemistry, University of Natural Resources and Life Sciences, Vienna, Konrad-Lorenz-Straße 24, 3430, Tulln, Austria
  2. Office of Safeguards Analytical Services, Department of Safeguards, International Atomic Energy Agency (IAEA), Vienna International Centre, PO Box 100, 1400, Vienna, Austria
  
• 刊物类别：Chemistry and Materials Science
• 刊物主题：Chemistry
  Analytical Chemistry
  Food Science
  Inorganic Chemistry
  Physical Chemistry
  Monitoring, Environmental Analysis and Environmental Ecotoxicology
  
• 出版者：Springer Berlin / Heidelberg
• ISSN：1618-2650

文摘

Laser ablation–multi-collector–inductively coupled plasma mass spectrometry (LA-MC-ICP-MS) was optimized and investigated with respect to its performance for determining spatially resolved Pu isotopic signatures within radioactive fuel particle clusters. Fuel particles had been emitted from the Chernobyl nuclear power plant (ChNPP) where the 1986 accident occurred and were deposited in the surrounding soil, where weathering processes caused their transformation into radioactive clusters, so-called micro-samples. The size of the investigated micro-samples, which showed surface alpha activities below 40 mBq, ranged from about 200 to 1000 μm. Direct single static point ablations allowed to identify variations of Pu isotopic signatures not only between distinct fuel particle clusters but also within individual clusters. The resolution was limited to 100 to 120 μm as a result of the applied laser ablation spot sizes and the resolving power of the nuclear track radiography methodology that was applied for particle pre-selection. The determined 242Pu/239Pu and 240Pu/239Pu isotope ratios showed a variation from low to high Pu isotope ratios, ranging from 0.007(2) to 0.047(8) for 242Pu/239Pu and from 0.183(13) to 0.577(40) for 240Pu/239Pu. In contrast to other studies, the applied methodology allowed for the first time to display the Pu isotopic distribution in the Chernobyl fallout, which reflects the differences in the spent fuel composition over the reactor core. The measured Pu isotopic signatures are in good agreement with the expected Pu isotopic composition distribution that is typical for a RBMK-1000 reactor, indicating that the analyzed samples are originating from the ill-fated Chernobyl reactor. The average Pu isotope ratios [240Pu/239Pu = 0.388(86), 242Pu/239Pu = 0.028(11)] that were calculated from all investigated samples (n = 48) correspond well to previously published results of Pu analyses in contaminated samples from the vicinity of the Chernobyl NPP [e.g. 240Pu/239Pu = 0.394(2) and 242Pu/239Pu = 0.027(1); Nunnemann et al. (J Alloys Compd 271–273:45–48, 1998)].