Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study
Abstract
This work presents the findings of a long term plutonium study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at Savannah River National Laboratory (SRNL) in A-area. Plutonium content and isotopic abundances were measured over this time period by alpha spectrometry and three stage thermal ionization mass spectrometry (3STIMS). Here we detail the complete sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the 238Pu/239+240Pu activity ratios attributed to SRS are above atmospheric global fallout ranges. The 240Pu/239Pu atom ratios are reasonably consistent from year to year and are lower than fallout, while the 242Pu/239Pu atom ratios are higher than fallout values. Overall, the plutonium signatures obtained in this study reflect a mixture of weapons-grade, higher burn-up, and fallout material. This study provides a blue print for long term low level monitoring of plutonium in the environment.
- Authors:
-
- Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)
- Publication Date:
- Research Org.:
- Savannah River Site (SRS), Aiken, SC (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1146964
- Report Number(s):
- SRNL-L2200-2014-00067
Journal ID: ISSN 0013-936X
- Grant/Contract Number:
- AC09-08SR22470
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 49; Journal Issue: 3; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES
Citation Formats
Armstrong, Christopher R., Nuessle, Patterson R., Brant, Heather A., Hall, Gregory, Halverson, Justin E., and Cadieux, James R. Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study. United States: N. p., 2015.
Web. doi:10.1021/es504147d.
Armstrong, Christopher R., Nuessle, Patterson R., Brant, Heather A., Hall, Gregory, Halverson, Justin E., & Cadieux, James R. Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study. United States. https://doi.org/10.1021/es504147d
Armstrong, Christopher R., Nuessle, Patterson R., Brant, Heather A., Hall, Gregory, Halverson, Justin E., and Cadieux, James R. Fri .
"Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study". United States. https://doi.org/10.1021/es504147d. https://www.osti.gov/servlets/purl/1146964.
@article{osti_1146964,
title = {Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study},
author = {Armstrong, Christopher R. and Nuessle, Patterson R. and Brant, Heather A. and Hall, Gregory and Halverson, Justin E. and Cadieux, James R.},
abstractNote = {This work presents the findings of a long term plutonium study at Savannah River Site (SRS) conducted between 2003 and 2013. Terrestrial environmental samples were obtained at Savannah River National Laboratory (SRNL) in A-area. Plutonium content and isotopic abundances were measured over this time period by alpha spectrometry and three stage thermal ionization mass spectrometry (3STIMS). Here we detail the complete sample collection, radiochemical separation, and measurement procedure specifically targeted to trace plutonium in bulk environmental samples. Total plutonium activities were determined to be not significantly above atmospheric global fallout. However, the 238Pu/239+240Pu activity ratios attributed to SRS are above atmospheric global fallout ranges. The 240Pu/239Pu atom ratios are reasonably consistent from year to year and are lower than fallout, while the 242Pu/239Pu atom ratios are higher than fallout values. Overall, the plutonium signatures obtained in this study reflect a mixture of weapons-grade, higher burn-up, and fallout material. This study provides a blue print for long term low level monitoring of plutonium in the environment.},
doi = {10.1021/es504147d},
journal = {Environmental Science and Technology},
number = 3,
volume = 49,
place = {United States},
year = {Fri Jan 16 00:00:00 EST 2015},
month = {Fri Jan 16 00:00:00 EST 2015}
}
Web of Science
Works referenced in this record:
Tracking the Fukushima Radionuclides
journal, May 2012
- Yoshida, N.; Kanda, J.
- Science, Vol. 336, Issue 6085
Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident
journal, March 2012
- Zheng, Jian; Tagami, Keiko; Watanabe, Yoshito
- Scientific Reports, Vol. 2, Issue 1
Fukushima’s Forgotten Radionuclides: A Review of the Understudied Radioactive Emissions
journal, April 2014
- Steinhauser, Georg
- Environmental Science & Technology, Vol. 48, Issue 9
Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations
journal, October 2013
- Schneider, Stephanie; Walther, Clemens; Bister, Stefan
- Scientific Reports, Vol. 3, Issue 1
Release of Plutonium Isotopes into the Environment from the Fukushima Daiichi Nuclear Power Plant Accident: What Is Known and What Needs to Be Known
journal, August 2013
- Zheng, Jian; Tagami, Keiko; Uchida, Shigeo
- Environmental Science & Technology, Vol. 47, Issue 17
Plutonium in the Savannah River Site Environment
journal, January 1996
- Carlton, W. H.; Murphy, C. E.; Evans, A. G.
- Health Physics, Vol. 71, Issue 3
Determination of plutonium from different sources in environmental samples using alpha-spectrometry and AMS
journal, April 2010
- Bisinger, T.; Hippler, S.; Michel, R.
- Nuclear Instruments and Methods in Physics Research Section B: Beam Interactions with Materials and Atoms, Vol. 268, Issue 7-8
Determination of acid leachable and total plutonium in large soil samples
journal, October 1987
- Krey, P. W.; Bogen, D. C.
- Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 115, Issue 2
Determination of plutonium isotopes and neptunium-237 in environmental samples by inductively coupled plasma mass spectrometry with total sample dissolution
journal, October 2002
- Kenna, Timothy C.
- Journal of Analytical Atomic Spectrometry, Vol. 17, Issue 11
Properties of ThO2 , UO2 and PuO2 as Function of Pretreatment and their Dissolution in HNO3.
journal, January 1984
- Greiling, H. -D.; Lieser, Κ. H.
- Radiochimica Acta, Vol. 35, Issue 2
The analysis of complex mixtures of elements resulting from the irradiation of fissile materials
journal, April 1956
- Crouch, E. A. C.; Cook, G. B.
- Journal of Inorganic and Nuclear Chemistry, Vol. 2, Issue 4
Electrodeposition of actinides for .alpha. spectrometric determination
journal, February 1972
- Talvitie, N. A.
- Analytical Chemistry, Vol. 44, Issue 2
Rapid separation and purification of uranium and plutonium from dilute-matrix samples
journal, March 2014
- Armstrong, Christopher R.; Ticknor, Brian W.; Hall, Gregory
- Journal of Radioanalytical and Nuclear Chemistry, Vol. 300, Issue 2
Plutonium from Mayak: Measurement of Isotope Ratios and Activities Using Accelerator Mass Spectrometry
journal, May 2000
- Oughton, Deborah H.; Fifield, L. Keith; Day, J. Philip
- Environmental Science & Technology, Vol. 34, Issue 10
Environmental study of fallout plutonium in soils from the piemonte region (North-West Italy)
journal, January 1987
- Cigna, Arrigo A.; Rossi, Luciana Cigna; Sgorbini, Sergio
- Journal of Environmental Radioactivity, Vol. 5, Issue 1
Mean residence time of plutonium in the troposphere
journal, February 1982
- Holloway, Robert W.; Hayes, David W.
- Environmental Science & Technology, Vol. 16, Issue 2
Plutonium, lead-210, and carbon isotopes in the Savannah estuary: riverborne versus marine sources
journal, December 1989
- Olsen, Curtis R.; Thein, Myint; Larsen, Ingvar L.
- Environmental Science & Technology, Vol. 23, Issue 12
The distribution of plutonium, Americium and curium isotopes in pond and stream sediments of the Savannah river plant, South Carolina, USA
journal, January 1986
- Alberts, J. J.; Halverson, J. E.; Orlandini, K. A.
- Journal of Environmental Radioactivity, Vol. 3, Issue 4
Investigations for isobaric interference of 238Pu at 238U during thermal ionization mass spectrometry of uranium and plutonium from the same filament loading
journal, December 1995
- Aggarwal, Suresh K.; Kumar, Sanjai; Saxena, Manoj K.
- International Journal of Mass Spectrometry and Ion Processes, Vol. 151, Issue 2-3
The geochemistry of fallout plutonium in the North Atlantic: II. ratios and their significance
journal, October 1987
- Buesseler, Ken O.; Sholkovitz, Edward R.
- Geochimica et Cosmochimica Acta, Vol. 51, Issue 10
A new ground-level fallout record of uranium and plutonium isotopes for northern temperate latitudes
journal, November 2002
- Warneke, Thorsten; Croudace, Ian W.; Warwick, Phillip E.
- Earth and Planetary Science Letters, Vol. 203, Issue 3-4
Perturbation in the 240Pu239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain)
journal, August 1997
- Mitchell, P. I.; Vintró, L. León; Dahlgaard, H.
- Science of The Total Environment, Vol. 202, Issue 1-3
Anomalous Plutonium Isotopic Ratios in Sediments of Lake Qinghai from the Qinghai-Tibetan Plateau, China
journal, November 2011
- Wu, Fengchang; Zheng, Jian; Liao, Haiqing
- Environmental Science & Technology, Vol. 45, Issue 21
Global distribution of Pu isotopes and 237Np
journal, September 1999
- Kelley, J. M.; Bond, L. A.; Beasley, T. M.
- Science of The Total Environment, Vol. 237-238
Long-term behaviour of plutonium in air and deposition and the role of resuspension in a semi-rural environment in Germany
journal, April 1997
- Rosner, G.; Hötzl, H.; Winkler, R.
- Science of The Total Environment, Vol. 196, Issue 3
Works referencing / citing this record:
Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope
journal, February 2016
- Armstrong, Christopher R.; Brant, Heather A.; Nuessle, Patterson R.
- Scientific Reports, Vol. 6, Issue 1