Safe and effective nuclear waste disposal, as well as accidental radionuclide releases, necessitates our understanding of the fate of radionuclides in the environment, including their interaction with microorganisms. We examined the sorption of Pu(IV) and Pu(V) to Pseudomonas sp. strain EPS-1W, an aerobic bacterium isolated from plutonium (Pu)-contaminated groundwater collected in the United States at the Nevada National Security Site (NNSS) in Nevada. We compared Pu sorption to cells with and without bound extracellular polymeric substances (EPS). Wild-type cells with intact EPS sorbed Pu(V) more effectively than cells with EPS removed. In contrast, cells with and without EPS showed the same sorption affinity for Pu(IV). In vitro experiments with extracted EPS revealed rapid reduction of Pu(V) to Pu(IV). Transmission electron microscopy indicated that 2-to 3-nm nanocrystalline Pu(IV)O 2 formed on cells equilibrated with high concentrations of Pu(IV) but not Pu(V). Thus, EPS, while facilitating Pu(V) reduction, inhibit the formation of nanocrystalline Pu(IV) precipitates.
IMPORTANCEOur results indicate that EPS are an effective reductant for Pu(V) and sorbent for Pu(IV) and may impact Pu redox cycling and mobility in the environment. Additionally, the resulting Pu morphology associated with EPS will depend on the concentration and initial Pu oxidation state. While our results are not directly applicable to the Pu transport situation at the NNSS, the results suggest that, in general, stationary microorganisms and biofilms will tend to limit the migration of Pu and provide an important Pu retardation mechanism in the environment. In a broader sense, our results, along with a growing body of literature, highlight the important role of microorganisms as producers of redox-active organic ligands and therefore as modulators of radionuclide redox transformations and complexation in the subsurface.T he civil production of nuclear energy and military production of nuclear materials have resulted in an estimated worldwide inventory of over 2,000 metric tons of plutonium (Pu) (1). This inventory continues to increase at a rate of approximately 70 metric tons per year as a result of global nuclear energy production (2). Due to its long half-life (24,100 years for 239 Pu) and high radiotoxicity (3), Pu is an important driver in public health risk assessments for nuclear waste repositories and radiologically contaminated sites. However, predicting how Pu behaves in the environment and ultimately calculating its human health risk are limited by our understanding of the dominant biogeochemical processes controlling its behavior.The behavior of Pu in the environment is strongly dependent on its oxidation state and concentration. Among all the actinides, Pu has one of the most complex chemical, redox, and surface sorption behaviors. At low concentrations, Pu can exist as aqueous species in the III, IV, V, and/or VI oxidation states, all of which have different solubilities (4), mineral sorption affinities (5-7), and hence...