Resolving Chernobyl vs. global fallout contributions in soils from Poland using Plutonium atom ratios measured by inductively coupled plasma mass spectrometry

Michael E. Ketterer, Kevin M. Hafer, Jerzy W. Mietelski

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Abstract

Plutonium in Polish forest soils and the Bór za Lasem peat bog is resolved between Chernobyl and global fallout contributions via inductively coupled plasma mass spectrometric measurements of 240Pu/ 239Pu and 241Pu/239Pu atom ratios in previously prepared NdF3 α spectrometric sources. Compared to global fallout, Chernobyl Pu exhibits higher abundances of 240Pu and 241Pu. The ratios 240Pu/239Pu and 241Pu/239Pu co-vary and range from 0.186 to 0.348 and 0.0029 to 0.0412, respectively, in forest soils (241Pu/ 239Pu=0.2407×[240Pu/239Pu]-0.0413; r 2=0.9924). Two-component mixing models are developed to ap portion 239+240Pu and 241Pu activities; various estimates of the percentage of Chernobyl-derived 239+240Pu activity in forest soils range from <10% to >90% for the sample set. The 240Pu/ 239Pu-241Pu/239Pu atom ratio mixing line extrapolates to estimate 241Pu/239Pu and the 241Pu/239+240Pu activity ratio for the Chernobyl source term (0.123±0.007; 83±5; 1 May 1986). Sample 241Pu activities, calculated using existing alpha spectrometric 239+240Pu activities, and the 240Pu/239Pu and 241Pu/ 239Pu atom ratios, agree relatively well with previous liquid scintillation spectrometry measurements. Chernobyl Pu is most evident in locations from northeastern Poland. The 241Pu activities and/or the 241Pu/239Pu atom ratios are more sensitive than 240Pu/239Pu or 238Pu/239+240Pu activity ratios at detecting small Chernobyl 239+240Pu inputs, found in southern Poland. The mass spectrometric data show that the 241Pu activity is 40-62% Chernobyl-derived in southern Poland, and 58-96% Chernobyl in northeastern Poland. The Bór za Lasem peat bog (49.42°N, 19.75°E), located in the Orawsko-Nowotarska valley of southern Poland, consists of global fallout Pu.

Original languageEnglish (US)
Pages (from-to)183-201
Number of pages19
JournalJournal of Environmental Radioactivity
Volume73
Issue number2
DOIs
StatePublished - Mar 24 2004

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Keywords

  • Chernobyl
  • Contamination
  • Inductively coupled plasma mass spectrometry
  • Isotopic ratios
  • Plutonium
  • Poland
  • Soils

ASJC Scopus subject areas

  • Environmental Chemistry
  • Waste Management and Disposal
  • Pollution
  • Health, Toxicology and Mutagenesis

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