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

Journal Article · · Scientific Reports
DOI:https://doi.org/10.1038/srep21512· OSTI ID:1252475
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  1. Savannah River Site (SRS), Aiken, SC (United States). Savannah River National Lab. (SRNL)

Owing to the rich history of heavy element production in the unique high flux reactors that operated at the Savannah River Site, USA (SRS) decades ago, trace quantities of plutonium with highly unique isotopic characteristics still persist today in the SRS terrestrial environment. Development of an effective sampling, processing, and analysis strategy enables detailed monitoring of the SRS environment, revealing plutonium isotopic compositions, e.g., 244Pu, that reflect the unique legacy of plutonium production at SRS. This work describes the first long-term investigation of anthropogenic 244Pu occurrence in the environment. Environmental samples, consisting of collected foot borne debris, were taken at SRS over an eleven year period, from 2003 to 2014. Separation and purification of trace plutonium was carried out followed by three stage thermal ionization mass spectrometry (3STIMS) measurements for plutonium isotopic content and isotopic ratios. Furthermore, significant 244Pu was measured in all of the years sampled with the highest amount observed in 2003. The 244Pu content, in femtograms (fg = 10–15 g) per gram, ranged from 0.31 fg/g to 44 fg/g in years 2006 and 2003 respectively. In all years, the 244Pu/239Pu atom ratios were significantly higher than global fallout, ranging from 0.003 to 0.698 in years 2014 and 2003 respectively.

Research Organization:
Savannah River Site (SRS), Aiken, SC (United States)
Sponsoring Organization:
USDOE
Grant/Contract Number:
AC09-08SR22470
OSTI ID:
1252475
Report Number(s):
SRNL-STI-2015-00194; srep21512
Journal Information:
Scientific Reports, Vol. 6, Issue 1; ISSN 2045-2322
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 7 works
Citation information provided by
Web of Science

References (29)

Plutonium Isotopes in the Terrestrial Environment at the Savannah River Site, USA: A Long-Term Study journal January 2015
Rare earth elements in chondritic phosphates—implications for 244Pu chronology journal November 1983
The iodine–plutonium–xenon age of the Moon–Earth system revisited journal September 2014
Plutonium-244 Fission Tracks: Evidence in a Lunar Rock 3.95 Billion Years Old journal May 1972
Frequency distribution, isotopic composition and physical characterization of plutonium-bearing particles from the Fig-Quince zone on Runit Island, Enewetak Atoll journal July 2009
The origin of the heavy elements: Recent progress in the understanding of the r-process journal January 2003
Extinct 244Pu in Ancient Zircons journal October 2004
Heavy Isotope Abundances in Mike Thermonuclear Device journal September 1960
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
A window on nucleosynthesis through detection of short-lived radionuclides journal May 2003
26Al, 244Pu, 50Ti, REE, and trace element abundances in hibonite grains from CM and CV meteorites journal February 1987
Plutonium from Mayak:  Measurement of Isotope Ratios and Activities Using Accelerator Mass Spectrometry journal May 2000
Rare gases in separated whitlockite from the St. Severin chondrite: xenon and krypton from fission of extinct 244Pu journal April 1975
Experimental Limit to Interstellar [TSUP]244[/TSUP]P[CLC]u[/CLC] Abundance journal September 2001
Nuclear Fission in the Early History of the Earth journal July 1960
Plutonium-244: Confirmation as an Extinct Radioactivity journal May 1971
Properties of ThO2 , UO2 and PuO2 as Function of Pretreatment and their Dissolution in HNO3. journal January 1984
Isotopic signature of plutonium at Bikini atoll journal June 2010
New Elements Einsteinium and Fermium, Atomic Numbers 99 and 100 journal August 1955
Abundance of live 244Pu in deep-sea reservoirs on Earth points to rarity of actinide nucleosynthesis journal January 2015
AMS of the Minor Plutonium Isotopes journal January 2013
Development of the NIST Rocky Flats Soil Standard journal April 2008
Supernova produced and anthropogenic 244Pu in deep sea manganese encrustations journal February 2004
The analysis of complex mixtures of elements resulting from the irradiation of fissile materials journal April 1956
Evaluation of Disposition Options for Mark-18A (Mk-18A) Target Materials report May 2013
Demonstration of Disposal of Americium and Curium Legacy Material Through High Level Waste System: Results from Baseline, Nitrate Added Flowsheet Studies report February 2002
Abundance of live ²⁴⁴Pu in deep-sea reservoirs on earth points to rarity of actinide nucleosynthesis text January 2015
New Elements Einsteinium and Fermium, Atomic Numbers 99 and 100 book May 1994
The iodine-plutonium-xenon age of the Moon-Earth system revisited text January 2015

Cited By (1)

241Pu in the environment: insight into the understudied isotope of plutonium journal June 2018