Resolving global versus local/regional Pu sources in the environment using sector ICP-MS

Michael E Ketterer, Kevin M. Hafer, Carolyn L. Link, Douglas Kolwaite, Jennifer Wilson, Jerzy W. Mietelski

Research output: Contribution to journalArticle

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Abstract

Sector inductively coupled plasma mass spectrometry is a versatile method for the determination of plutonium activities and isotopic compositions in samples containing this element at fallout levels. Typical detection limits for 239+240Pu are 0.1, 0.02 and 0.002 Bq kg -1Pu for samples sizes of 0.5 g, 3 g, and 50 g of soil, respectively. The application of sector ICP-MS-based Pu determinations is demonstrated in studies in sediment chronology, soil Pu inventory and depth distribution, and the provenance of global fallout versus local or regional Pu sources. A sediment core collected from Sloans Lake (Denver, Colorado, USA) exhibits very similar 137Cs and 239+240Pu activity profiles; 240Pu/239Pu atom ratios indicate possible small influences from the Nevada Test Site and/or the Rocky Flats Environmental Technology Site. An undisturbed soil profile from Lockett Meadow (Flagstaff, Arizona, USA) exhibits an exponential decrease in 239+240Pu activity versus depth; 240Pu/239Pu in the top 3 cm is slightly lower than the global fallout range of 0.180 ± 0.014 due to possible regional influence of Nevada Test Site fallout. The 239±240Pu inventory at Lockett Meadow is 56 ± 4 Bq m-2, consistent with Northern Hemisphere mid-latitude fallout. Archived NdF3 sources, prepared from Polish soils, demonstrate that substantial 239+240Pu from the 1986 Chernobyl disaster has been deposited in north eastern regions of Poland; 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 0.186-0.348 and 0.0029-0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407·[240Pu/239Pu] - 0.0413; r2 = 0.9924).

Original languageEnglish (US)
Pages (from-to)241-245
Number of pages5
JournalJournal of Analytical Atomic Spectrometry
Volume19
Issue number2
DOIs
StatePublished - 2004

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Fallout
Inductively coupled plasma
Soils
Sediments
Environmental technology
Plutonium
Inductively coupled plasma mass spectrometry
Disasters
Lakes
Atoms
Chemical analysis

ASJC Scopus subject areas

  • Spectroscopy

Cite this

Resolving global versus local/regional Pu sources in the environment using sector ICP-MS. / Ketterer, Michael E; Hafer, Kevin M.; Link, Carolyn L.; Kolwaite, Douglas; Wilson, Jennifer; Mietelski, Jerzy W.

In: Journal of Analytical Atomic Spectrometry, Vol. 19, No. 2, 2004, p. 241-245.

Research output: Contribution to journalArticle

Ketterer, Michael E ; Hafer, Kevin M. ; Link, Carolyn L. ; Kolwaite, Douglas ; Wilson, Jennifer ; Mietelski, Jerzy W. / Resolving global versus local/regional Pu sources in the environment using sector ICP-MS. In: Journal of Analytical Atomic Spectrometry. 2004 ; Vol. 19, No. 2. pp. 241-245.
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abstract = "Sector inductively coupled plasma mass spectrometry is a versatile method for the determination of plutonium activities and isotopic compositions in samples containing this element at fallout levels. Typical detection limits for 239+240Pu are 0.1, 0.02 and 0.002 Bq kg -1Pu for samples sizes of 0.5 g, 3 g, and 50 g of soil, respectively. The application of sector ICP-MS-based Pu determinations is demonstrated in studies in sediment chronology, soil Pu inventory and depth distribution, and the provenance of global fallout versus local or regional Pu sources. A sediment core collected from Sloans Lake (Denver, Colorado, USA) exhibits very similar 137Cs and 239+240Pu activity profiles; 240Pu/239Pu atom ratios indicate possible small influences from the Nevada Test Site and/or the Rocky Flats Environmental Technology Site. An undisturbed soil profile from Lockett Meadow (Flagstaff, Arizona, USA) exhibits an exponential decrease in 239+240Pu activity versus depth; 240Pu/239Pu in the top 3 cm is slightly lower than the global fallout range of 0.180 ± 0.014 due to possible regional influence of Nevada Test Site fallout. The 239±240Pu inventory at Lockett Meadow is 56 ± 4 Bq m-2, consistent with Northern Hemisphere mid-latitude fallout. Archived NdF3 sources, prepared from Polish soils, demonstrate that substantial 239+240Pu from the 1986 Chernobyl disaster has been deposited in north eastern regions of Poland; 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 0.186-0.348 and 0.0029-0.0412, respectively, in forest soils (241Pu/239Pu = 0.2407·[240Pu/239Pu] - 0.0413; r2 = 0.9924).",
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