Anthropogenic 236U at Rocky Flats, Ashtabula river harbor, and Mersey estuary

Three case studies by sector inductively coupled plasma mass spectrometry

Michael E Ketterer, K. M. Hafer, C. L. Link, C. S. Royden, W. J. Hartsock

Research output: Contribution to journalArticle

37 Citations (Scopus)

Abstract

236U (t1/2=2.3×107 y) is formed as a result of thermal neutron capture by 235U. In naturally occurring U ores, where a high neutron flux is present from spontaneous fission of 238U, 236U/238U atom ratios are ∼10-4 ppm. In the natural Earth's crust, unaffected by nuclear fallout, these ratios are expected to be on the order of 10-8 ppm. Reactor-irradiated U, however, exhibits high 236U/238U atom ratios approaching 104 ppm. As a result, the presence of very small quantities of reactor-irradiated U will significantly enhance the 'background' 236U/238U atom ratio. When sufficiently elevated 236U/238U ratios are present, the determination of 236U/238U by rapid inductively coupled plasma mass spectrometric (ICPMS) methods is attractive. We have used sector ICPMS at medium resolving power (R=3440) to measure 236U/238U atom ratios with a determination limit of 0.2 ppm. The limiting factors in the measurement are the 235U1H+ isobar and background signal at m/z 236 arising from the 238U+ peak tail. Based upon the analysis of replicates and considerations of possible systematic errors, uncertainties of ±5% are found for 236U/238U atom ratios of 1-100 ppm. This procedure has been demonstrated in studies of anthropogenic 236U in the environment at three locations: (a) offsite soils from the vicinity of the Rocky Flats Environmental Technology site (Golden, Colorado, USA); (b) sediments from the Ashtabula River (Ohio, USA); and (c) sediments from the Mersey estuary (Liverpool, UK). In each of these three locations, definite plumes of elevated 236U/238U are identified and characterized. Maximum 236U/238U atom ratios observed in RFETS-vicinity soils, the Ashtabula River, and the Mersey Estuary are 2.8, 140, and 4.4 ppm, respectively.

Original languageEnglish (US)
Pages (from-to)191-206
Number of pages16
JournalJournal of Environmental Radioactivity
Volume67
Issue number3
DOIs
StatePublished - 2003

Fingerprint

Inductively coupled plasma mass spectrometry
Estuaries
Neutrons
Ports and harbors
Rivers
Mass Spectrometry
harbor
Soil
mass spectrometry
estuary
plasma
environmental technology
Atoms
fallout
river
limiting factor
sediment
Uncertainty
soil
plume

Keywords

  • U
  • Ashtabula
  • Contamination
  • Inductively coupled plasma mass spectrometry
  • Mersey estuary
  • Plutonium
  • Rocky flats
  • Sediments
  • Uranium

ASJC Scopus subject areas

  • Environmental Science(all)

Cite this

Anthropogenic 236U at Rocky Flats, Ashtabula river harbor, and Mersey estuary : Three case studies by sector inductively coupled plasma mass spectrometry. / Ketterer, Michael E; Hafer, K. M.; Link, C. L.; Royden, C. S.; Hartsock, W. J.

In: Journal of Environmental Radioactivity, Vol. 67, No. 3, 2003, p. 191-206.

Research output: Contribution to journalArticle

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abstract = "236U (t1/2=2.3×107 y) is formed as a result of thermal neutron capture by 235U. In naturally occurring U ores, where a high neutron flux is present from spontaneous fission of 238U, 236U/238U atom ratios are ∼10-4 ppm. In the natural Earth's crust, unaffected by nuclear fallout, these ratios are expected to be on the order of 10-8 ppm. Reactor-irradiated U, however, exhibits high 236U/238U atom ratios approaching 104 ppm. As a result, the presence of very small quantities of reactor-irradiated U will significantly enhance the 'background' 236U/238U atom ratio. When sufficiently elevated 236U/238U ratios are present, the determination of 236U/238U by rapid inductively coupled plasma mass spectrometric (ICPMS) methods is attractive. We have used sector ICPMS at medium resolving power (R=3440) to measure 236U/238U atom ratios with a determination limit of 0.2 ppm. The limiting factors in the measurement are the 235U1H+ isobar and background signal at m/z 236 arising from the 238U+ peak tail. Based upon the analysis of replicates and considerations of possible systematic errors, uncertainties of ±5{\%} are found for 236U/238U atom ratios of 1-100 ppm. This procedure has been demonstrated in studies of anthropogenic 236U in the environment at three locations: (a) offsite soils from the vicinity of the Rocky Flats Environmental Technology site (Golden, Colorado, USA); (b) sediments from the Ashtabula River (Ohio, USA); and (c) sediments from the Mersey estuary (Liverpool, UK). In each of these three locations, definite plumes of elevated 236U/238U are identified and characterized. Maximum 236U/238U atom ratios observed in RFETS-vicinity soils, the Ashtabula River, and the Mersey Estuary are 2.8, 140, and 4.4 ppm, respectively.",
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T2 - Three case studies by sector inductively coupled plasma mass spectrometry

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AU - Link, C. L.

AU - Royden, C. S.

AU - Hartsock, W. J.

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N2 - 236U (t1/2=2.3×107 y) is formed as a result of thermal neutron capture by 235U. In naturally occurring U ores, where a high neutron flux is present from spontaneous fission of 238U, 236U/238U atom ratios are ∼10-4 ppm. In the natural Earth's crust, unaffected by nuclear fallout, these ratios are expected to be on the order of 10-8 ppm. Reactor-irradiated U, however, exhibits high 236U/238U atom ratios approaching 104 ppm. As a result, the presence of very small quantities of reactor-irradiated U will significantly enhance the 'background' 236U/238U atom ratio. When sufficiently elevated 236U/238U ratios are present, the determination of 236U/238U by rapid inductively coupled plasma mass spectrometric (ICPMS) methods is attractive. We have used sector ICPMS at medium resolving power (R=3440) to measure 236U/238U atom ratios with a determination limit of 0.2 ppm. The limiting factors in the measurement are the 235U1H+ isobar and background signal at m/z 236 arising from the 238U+ peak tail. Based upon the analysis of replicates and considerations of possible systematic errors, uncertainties of ±5% are found for 236U/238U atom ratios of 1-100 ppm. This procedure has been demonstrated in studies of anthropogenic 236U in the environment at three locations: (a) offsite soils from the vicinity of the Rocky Flats Environmental Technology site (Golden, Colorado, USA); (b) sediments from the Ashtabula River (Ohio, USA); and (c) sediments from the Mersey estuary (Liverpool, UK). In each of these three locations, definite plumes of elevated 236U/238U are identified and characterized. Maximum 236U/238U atom ratios observed in RFETS-vicinity soils, the Ashtabula River, and the Mersey Estuary are 2.8, 140, and 4.4 ppm, respectively.

AB - 236U (t1/2=2.3×107 y) is formed as a result of thermal neutron capture by 235U. In naturally occurring U ores, where a high neutron flux is present from spontaneous fission of 238U, 236U/238U atom ratios are ∼10-4 ppm. In the natural Earth's crust, unaffected by nuclear fallout, these ratios are expected to be on the order of 10-8 ppm. Reactor-irradiated U, however, exhibits high 236U/238U atom ratios approaching 104 ppm. As a result, the presence of very small quantities of reactor-irradiated U will significantly enhance the 'background' 236U/238U atom ratio. When sufficiently elevated 236U/238U ratios are present, the determination of 236U/238U by rapid inductively coupled plasma mass spectrometric (ICPMS) methods is attractive. We have used sector ICPMS at medium resolving power (R=3440) to measure 236U/238U atom ratios with a determination limit of 0.2 ppm. The limiting factors in the measurement are the 235U1H+ isobar and background signal at m/z 236 arising from the 238U+ peak tail. Based upon the analysis of replicates and considerations of possible systematic errors, uncertainties of ±5% are found for 236U/238U atom ratios of 1-100 ppm. This procedure has been demonstrated in studies of anthropogenic 236U in the environment at three locations: (a) offsite soils from the vicinity of the Rocky Flats Environmental Technology site (Golden, Colorado, USA); (b) sediments from the Ashtabula River (Ohio, USA); and (c) sediments from the Mersey estuary (Liverpool, UK). In each of these three locations, definite plumes of elevated 236U/238U are identified and characterized. Maximum 236U/238U atom ratios observed in RFETS-vicinity soils, the Ashtabula River, and the Mersey Estuary are 2.8, 140, and 4.4 ppm, respectively.

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