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

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

doi:10.1038/srep21512

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

Journal Article · Mon Feb 22 00:00:00 EST 2016 · Scientific Reports

DOI:https://doi.org/10.1038/srep21512· OSTI ID:1252475

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

View Accepted Manuscript (DOE)

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, Journal Name: Scientific Reports Journal Issue: 1 Vol. 6; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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