Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)

Balboni, Enrica; Merino, Nancy; Begg, James D.; Samperton, Kyle M.; Zengotita, Frances E.; Law, Gareth T. W.; Kersting, Annie B.; Zavarin, Mavrik

doi:10.1016/j.chemosphere.2022.136240

Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)

Journal Article · Wed Aug 31 00:00:00 EDT 2022 · Chemosphere

DOI:https://doi.org/10.1016/j.chemosphere.2022.136240· OSTI ID:2008183

^[1]; ^[1]; ^[2]; ^[3]; ^[4]; Law, Gareth T. W. ^[5]; ^[1]; Zavarin, Mavrik ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Amphos 21, Barcelona (Spain)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Savannah River National Laboratory (SRNL), Aiken, SC (United States)
Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); University of Notre Dame, IN (United States)
Univ. of Helsinki (Finland)

Since 1952, liquid radioactive effluent containing^238-242Pu, ²⁴¹Am, ²³⁷Np, ¹³⁷Cs, and ⁹⁹Tc has been released with authorization from the Sellafield nuclear complex (UK) into the Irish Sea. This represents the largest source of plutonium (Pu) discharged in all western Europe, with 276 kg having been released. In the Eastern Irish Sea, the majority of the transuranic activity has settled into an area of sediments (Mudpatch) located off the Cumbrian coast. Radionuclides from the Mudpatch have been re-dispersed via particulate transport in fine-grained estuarine and intertidal sediments to the North-East Irish Sea, including the intertidal saltmarsh located at the mouth of the Esk Estuary. Saltmarshes are highly dynamic systems which are vulnerable to external agents (sea level change, erosion, sediment supply, and freshwater inputs), and their stability remains uncertain under current sea level rise projections and possible increases in storm activity. In this work, we examined factors affecting Pu mobility in contaminated sediments collected from the Esk Estuary by conducting leaching experiments under both anoxic and oxic conditions. Here, leaching experiments were conducted over a 9-month period and were periodically sampled to determine solution phase Pu via multicollector-inductively coupled plasma-mass spectrometry (MC-ICP-MS), and to measure redox indicators (Eh, pH and extractable Fe(II)). Microbial community composition was also characterized in the sediments, and at the beginning and end of the anoxic/oxic experiments. Results show that: 1) Pu leaching is about three times greater in solutions leached under anoxic conditions compared to oxic conditions, 2) the sediment slurry microbial communities shift as conditions change from anoxic to oxic, 3) Pu leaching is enhanced in the shallow sediments (0–10 cm depth), and 4) the magnitude of Pu leached from sediments is not correlated with total Pu, indicating that the biogeochemistry of sediment-associated Pu is spatially heterogeneous. These findings provide constraints on the stability of redox sensitive Pu in biogeochemically dynamic/transient environments on a timescale of months and suggests that anoxic conditions can enhance Pu mobility in estuarine systems.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States); Savannah River National Laboratory (SRNL), Aiken, SC (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: 89303321CEM000080; AC52-07NA27344

OSTI ID:: 2008183

Report Number(s):: LLNL--JRNL-831425; 1048284

Journal Information:: Chemosphere, Journal Name: Chemosphere Vol. 308; ISSN 0045-6535

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Thesis/Dissertation · Mon Dec 31 23:00:00 EST 1984 · OSTI ID:6069130

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38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY
Irish sea
anoxic conditions
contaminated sediments
microbial communities
plutonium
plutonium leaching
redox chemistry

Plutonium mobilization from contaminated estuarine sediments, Esk Estuary (UK)

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