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Title: Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site

Journal Article · · Radiochimica Acta, 102(12):1059-1068

The occurrence of plutonium dioxide (PuO2) either from direct deposition or from the precipitation of plutonium-bearing solutions in contaminated soils and sediments has been well described, particularly for the Hanford site in Washington State. However, past research has suggested that plutonium may exist in environmental samples at the Hanford site in chemical forms in addition to large size PuO2 particles and that these previously unidentified nano-sized particles maybe more reactive and thus more likely to influence the environmental mobility of Pu. Here we present evidence for the formation of nano-sized plutonium iron phosphate hydroxide structurally related to the rhabdophane group nanoparticles in 216-Z9 crib sediments from Hanford using transmission electron microscopy (TEM). The distribution and nature of these nanoparticles varied depending on the adjacent phases present. Fine electron probes were used to obtain electron diffraction and electron energy-loss spectra from specific phase regions of the 216-Z9 cribs specimens from fine-grained plutonium oxide and phosphate phases. Energy-loss spectra were used to evaluate the plutonium N4,5 (4d → 5f ) and iron L2,3 absorption edges. The iron plutonium phosphate formation may depend on the local micro-environment in the sediments, availability of phosphate, and hence the distribution of these minerals may control long-term migration of Pu in the soil. This study also points to the utility of using electron beam methods for determining the identity of actinide phases and their association with other sediment phases.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States). Environmental Molecular Sciences Lab. (EMSL)
Sponsoring Organization:
USDOE
DOE Contract Number:
AC05-76RL01830
OSTI ID:
1170453
Report Number(s):
PNNL-SA-90264; 42318; KP1702030
Journal Information:
Radiochimica Acta, 102(12):1059-1068, Journal Name: Radiochimica Acta, 102(12):1059-1068
Country of Publication:
United States
Language:
English