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

Abstract

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-termmore » 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.« less

Authors:
; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1170453
Report Number(s):
PNNL-SA-90264
42318; KP1702030
DOE Contract Number:
AC05-76RL01830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Radiochimica Acta, 102(12):1059-1068
Country of Publication:
United States
Language:
English
Subject:
Electron Energy-Loss Spectroscopy; Transmission Electron Microscopy; Plutonium; Hanford Site; Cribs, Soil Contamination; Plutonium Phosphate; Environmental Molecular Sciences Laboratory

Citation Formats

Buck, Edgar C., Moore, Dean A., Czerwinski, Kenneth R., Conradson, Steven D., Batuk, Olga, and Felmy, Andrew R.. Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site. United States: N. p., 2014. Web. doi:10.1515/ract-2013-2103.
Buck, Edgar C., Moore, Dean A., Czerwinski, Kenneth R., Conradson, Steven D., Batuk, Olga, & Felmy, Andrew R.. Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site. United States. doi:10.1515/ract-2013-2103.
Buck, Edgar C., Moore, Dean A., Czerwinski, Kenneth R., Conradson, Steven D., Batuk, Olga, and Felmy, Andrew R.. Wed . "Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site". United States. doi:10.1515/ract-2013-2103.
@article{osti_1170453,
title = {Nature of Nano-Sized Plutonium Particles in Soils at the Hanford Site},
author = {Buck, Edgar C. and Moore, Dean A. and Czerwinski, Kenneth R. and Conradson, Steven D. and Batuk, Olga and Felmy, Andrew R.},
abstractNote = {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.},
doi = {10.1515/ract-2013-2103},
journal = {Radiochimica Acta, 102(12):1059-1068},
number = ,
volume = ,
place = {United States},
year = {Wed Aug 06 00:00:00 EDT 2014},
month = {Wed Aug 06 00:00:00 EDT 2014}
}
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