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 - 2004

Fingerprint

Plutonium
Fallout
Inductively coupled plasma mass spectrometry
plutonium
Poland
fallout
forest soil
Mass Spectrometry
Soil
mass spectrometry
Soils
peatland
plasma
Atoms
Peat
Wetlands
soil
mixing ratio
spectrometry
Inductively coupled plasma

Keywords

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

ASJC Scopus subject areas

  • Environmental Science(all)

Cite this

@article{5c494d4dfd744e07b5fb00e1fff79df1,
title = "Resolving Chernobyl vs. global fallout contributions in soils from Poland using Plutonium atom ratios measured by inductively coupled plasma mass spectrometry",
abstract = "Plutonium in Polish forest soils and the B{\'o}r 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 B{\'o}r za Lasem peat bog (49.42°N, 19.75°E), located in the Orawsko-Nowotarska valley of southern Poland, consists of global fallout Pu.",
keywords = "Chernobyl, Contamination, Inductively coupled plasma mass spectrometry, Isotopic ratios, Plutonium, Poland, Soils",
author = "Ketterer, {Michael E} and Hafer, {Kevin M.} and Mietelski, {Jerzy W.}",
year = "2004",
doi = "10.1016/j.jenvrad.2003.09.001",
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volume = "73",
pages = "183--201",
journal = "Journal of Environmental Radioactivity",
issn = "0265-931X",
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TY - JOUR

T1 - Resolving Chernobyl vs. global fallout contributions in soils from Poland using Plutonium atom ratios measured by inductively coupled plasma mass spectrometry

AU - Ketterer, Michael E

AU - Hafer, Kevin M.

AU - Mietelski, Jerzy W.

PY - 2004

Y1 - 2004

N2 - 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.

AB - 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.

KW - Chernobyl

KW - Contamination

KW - Inductively coupled plasma mass spectrometry

KW - Isotopic ratios

KW - Plutonium

KW - Poland

KW - Soils

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U2 - 10.1016/j.jenvrad.2003.09.001

DO - 10.1016/j.jenvrad.2003.09.001

M3 - Article

C2 - 15023447

AN - SCOPUS:1542411344

VL - 73

SP - 183

EP - 201

JO - Journal of Environmental Radioactivity

JF - Journal of Environmental Radioactivity

SN - 0265-931X

IS - 2

ER -