Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study

Armstrong, Christopher R.; Nuessle, Patterson R.; Brant, Heather A.; Hall, Gregory; Halverson, Justin E.; Cadieux, James R.

doi:10.1021/es504147d

Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study

Journal Article · Fri Jan 16 00:00:00 EST 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/es504147d· OSTI ID:1146964

Armstrong, Christopher R. ^[1]; Nuessle, Patterson R. ^[1]; Brant, Heather A. ^[1]; Hall, Gregory ^[1]; Halverson, Justin E. ^[1]; Cadieux, James R. ^[1]

Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

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.

View Accepted Manuscript (DOE)

Research Organization:: Savannah River Site (SRS), Aiken, SC (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC09-08SR22470

OSTI ID:: 1146964

Report Number(s):: SRNL--L2200-2014-00067

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 3 Vol. 49; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

References (25)

Determination of acid leachable and total plutonium in large soil samples Krey, P. W.; Bogen, D. C. Journal of Radioanalytical and Nuclear Chemistry Articles, Vol. 115, Issue 2 https://doi.org/10.1007/BF02037448	journal	October 1987
Rapid separation and purification of uranium and plutonium from dilute-matrix samples Armstrong, Christopher R.; Ticknor, Brian W.; Hall, Gregory Journal of Radioanalytical and Nuclear Chemistry, Vol. 300, Issue 2 https://doi.org/10.1007/s10967-014-3070-9	journal	March 2014
The geochemistry of fallout plutonium in the North Atlantic: II. ratios and their significance Buesseler, Ken O.; Sholkovitz, Edward R. Geochimica et Cosmochimica Acta, Vol. 51, Issue 10 https://doi.org/10.1016/0016-7037(87)90144-X	journal	October 1987
The analysis of complex mixtures of elements resulting from the irradiation of fissile materials Crouch, E. A. C.; Cook, G. B. Journal of Inorganic and Nuclear Chemistry, Vol. 2, Issue 4 https://doi.org/10.1016/0022-1902(56)80048-1	journal	April 1956
Investigations for isobaric interference of 238Pu at 238U during thermal ionization mass spectrometry of uranium and plutonium from the same filament loading Aggarwal, Suresh K.; Kumar, Sanjai; Saxena, Manoj K. International Journal of Mass Spectrometry and Ion Processes, Vol. 151, Issue 2-3 https://doi.org/10.1016/0168-1176(95)04316-0	journal	December 1995
The distribution of plutonium, Americium and curium isotopes in pond and stream sediments of the Savannah river plant, South Carolina, USA Alberts, J. J.; Halverson, J. E.; Orlandini, K. A. Journal of Environmental Radioactivity, Vol. 3, Issue 4 https://doi.org/10.1016/0265-931X(86)90002-0	journal	January 1986
Environmental study of fallout plutonium in soils from the piemonte region (North-West Italy) Cigna, Arrigo A.; Rossi, Luciana Cigna; Sgorbini, Sergio Journal of Environmental Radioactivity, Vol. 5, Issue 1 https://doi.org/10.1016/0265-931X(87)90045-2	journal	January 1987
A new ground-level fallout record of uranium and plutonium isotopes for northern temperate latitudes Warneke, Thorsten; Croudace, Ian W.; Warwick, Phillip E. Earth and Planetary Science Letters, Vol. 203, Issue 3-4 https://doi.org/10.1016/S0012-821X(02)00930-5	journal	November 2002
Perturbation in the 240Pu239Pu global fallout ratio in local sediments following the nuclear accidents at Thule (Greenland) and Palomares (Spain) Mitchell, P. I.; Vintró, L. León; Dahlgaard, H. Science of The Total Environment, Vol. 202, Issue 1-3 https://doi.org/10.1016/S0048-9697(97)00111-3	journal	August 1997
Long-term behaviour of plutonium in air and deposition and the role of resuspension in a semi-rural environment in Germany Rosner, G.; Hötzl, H.; Winkler, R. Science of The Total Environment, Vol. 196, Issue 3 https://doi.org/10.1016/S0048-9697(97)05427-2	journal	April 1997
Global distribution of Pu isotopes and 237Np Kelley, J. M.; Bond, L. A.; Beasley, T. M. Science of The Total Environment, Vol. 237-238 https://doi.org/10.1016/S0048-9697(99)00160-6	journal	September 1999
Determination of plutonium from different sources in environmental samples using alpha-spectrometry and AMS 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 https://doi.org/10.1016/j.nimb.2009.10.150	journal	April 2010
Electrodeposition of actinides for .alpha. spectrometric determination Talvitie, N. A. Analytical Chemistry, Vol. 44, Issue 2 https://doi.org/10.1021/ac60310a013	journal	February 1972
Plutonium, lead-210, and carbon isotopes in the Savannah estuary: riverborne versus marine sources Olsen, Curtis R.; Thein, Myint; Larsen, Ingvar L. Environmental Science & Technology, Vol. 23, Issue 12 https://doi.org/10.1021/es00070a004	journal	December 1989
Mean residence time of plutonium in the troposphere Holloway, Robert W.; Hayes, David W. Environmental Science & Technology, Vol. 16, Issue 2 https://doi.org/10.1021/es00096a015	journal	February 1982
Anomalous Plutonium Isotopic Ratios in Sediments of Lake Qinghai from the Qinghai-Tibetan Plateau, China Wu, Fengchang; Zheng, Jian; Liao, Haiqing Environmental Science & Technology, Vol. 45, Issue 21 https://doi.org/10.1021/es202315c	journal	November 2011
Release of Plutonium Isotopes into the Environment from the Fukushima Daiichi Nuclear Power Plant Accident: What Is Known and What Needs to Be Known Zheng, Jian; Tagami, Keiko; Uchida, Shigeo Environmental Science & Technology, Vol. 47, Issue 17 https://doi.org/10.1021/es402212v	journal	August 2013
Fukushima’s Forgotten Radionuclides: A Review of the Understudied Radioactive Emissions Steinhauser, Georg Environmental Science & Technology, Vol. 48, Issue 9 https://doi.org/10.1021/es405654c	journal	April 2014
Plutonium from Mayak: Measurement of Isotope Ratios and Activities Using Accelerator Mass Spectrometry Oughton, Deborah H.; Fifield, L. Keith; Day, J. Philip Environmental Science & Technology, Vol. 34, Issue 10 https://doi.org/10.1021/es990847z	journal	May 2000
Isotopic evidence of plutonium release into the environment from the Fukushima DNPP accident Zheng, Jian; Tagami, Keiko; Watanabe, Yoshito Scientific Reports, Vol. 2, Issue 1 https://doi.org/10.1038/srep00304	journal	March 2012
Plutonium release from Fukushima Daiichi fosters the need for more detailed investigations Schneider, Stephanie; Walther, Clemens; Bister, Stefan Scientific Reports, Vol. 3, Issue 1 https://doi.org/10.1038/srep02988	journal	October 2013
Determination of plutonium isotopes and neptunium-237 in environmental samples by inductively coupled plasma mass spectrometry with total sample dissolution Kenna, Timothy C. Journal of Analytical Atomic Spectrometry, Vol. 17, Issue 11 https://doi.org/10.1039/b205001c	journal	October 2002
Plutonium in the Savannah River Site Environment Carlton, W. H.; Murphy, C. E.; Evans, A. G. Health Physics, Vol. 71, Issue 3 https://doi.org/10.1097/00004032-199609000-00004	journal	January 1996
Tracking the Fukushima Radionuclides Yoshida, N.; Kanda, J. Science, Vol. 336, Issue 6085 https://doi.org/10.1126/science.1219493	journal	May 2012
Properties of ThO2 , UO2 and PuO2 as Function of Pretreatment and their Dissolution in HNO3. Greiling, H. -D.; Lieser, Κ. H. Radiochimica Acta, Vol. 35, Issue 2 https://doi.org/10.1524/ract.1984.35.2.79	journal	January 1984

Cited By (1)

Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope Armstrong, Christopher R.; Brant, Heather A.; Nuessle, Patterson R. Scientific Reports, Vol. 6, Issue 1 https://doi.org/10.1038/srep21512	journal	February 2016

Similar Records

Anthropogenic plutonium-244 in the environment: Insights into plutonium’s longest-lived isotope

Journal Article · Sun Feb 21 19:00:00 EST 2016 · Scientific Reports · OSTI ID:1252475

Plutonium isotope ratio variations in North America

Conference · Mon Dec 13 23:00:00 EST 2010 · OSTI ID:1044154

Determination of Plutonium Activity Concentrations and 240Pu/239Pu Atom Ratios in Brown Algae (Fucus distichus) Collected from Amchitka Island, Alaska.

Technical Report · Mon May 02 00:00:00 EDT 2005 · OSTI ID:15016341

Related Subjects

54 ENVIRONMENTAL SCIENCES

Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA. A Long-Term Study

Citation Formats

References (25)

Cited By (1)

Similar Records

Related Subjects