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Title: Controls on Soluble Pu Concentrations in PuO2/Magnetite Suspensions

Abstract

Time-dependent reduction of PuO2(am) was studied over a range of pH values in the presence of aqueous Fe(II) and magnetite (Fe3O4) nanoparticles. At early time frames (up to 56 days) very little aqueous Pu was mobilized from PuO2(am), even though measured pH and redox potentials, coupled to equilibrium thermodynamic modeling indicated the potential for significant reduction of PuO2(am) to relatively soluble Pu(III). Introduction of Eu(III) or Nd(III) to the suspensions as competitive cations to displace possible sorbed Pu(III) resulted in the release of significant concentrations of aqueous Pu. However, the similarity of aqueous Pu concentrations that resulted from the introduction of Eu(III)/Nd(III) to suspensions with and without magnetite indicated that the Pu was displaced from the PuO2(am), not from magnetite. The fact that soluble forms of Pu can be displaced from the surface of PuO2(am) represents a potential, but previously unidentified, source of Pu to aqueous solution or subsurface groundwaters.

Authors:
; ; ; ; ; ; ;
Publication Date:
Research Org.:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US), Environmental Molecular Sciences Laboratory (EMSL)
Sponsoring Org.:
USDOE
OSTI Identifier:
1059612
Report Number(s):
PNNL-SA-83931
42318; KP1702030
DOE Contract Number:  
AC05-76RL01830
Resource Type:
Journal Article
Journal Name:
Environmental Science & Technology, 46(21):11610-11617
Additional Journal Information:
Journal Name: Environmental Science & Technology, 46(21):11610-11617
Country of Publication:
United States
Language:
English
Subject:
Environmental Molecular Sciences Laboratory

Citation Formats

Felmy, Andrew R., Moore, Dean A., Pearce, Carolyn I., Conradson, Steven D., Qafoku, Odeta, Buck, Edgar C., Rosso, Kevin M., and Ilton, Eugene S. Controls on Soluble Pu Concentrations in PuO2/Magnetite Suspensions. United States: N. p., 2012. Web. doi:10.1021/es3028956.
Felmy, Andrew R., Moore, Dean A., Pearce, Carolyn I., Conradson, Steven D., Qafoku, Odeta, Buck, Edgar C., Rosso, Kevin M., & Ilton, Eugene S. Controls on Soluble Pu Concentrations in PuO2/Magnetite Suspensions. United States. doi:10.1021/es3028956.
Felmy, Andrew R., Moore, Dean A., Pearce, Carolyn I., Conradson, Steven D., Qafoku, Odeta, Buck, Edgar C., Rosso, Kevin M., and Ilton, Eugene S. Tue . "Controls on Soluble Pu Concentrations in PuO2/Magnetite Suspensions". United States. doi:10.1021/es3028956.
@article{osti_1059612,
title = {Controls on Soluble Pu Concentrations in PuO2/Magnetite Suspensions},
author = {Felmy, Andrew R. and Moore, Dean A. and Pearce, Carolyn I. and Conradson, Steven D. and Qafoku, Odeta and Buck, Edgar C. and Rosso, Kevin M. and Ilton, Eugene S.},
abstractNote = {Time-dependent reduction of PuO2(am) was studied over a range of pH values in the presence of aqueous Fe(II) and magnetite (Fe3O4) nanoparticles. At early time frames (up to 56 days) very little aqueous Pu was mobilized from PuO2(am), even though measured pH and redox potentials, coupled to equilibrium thermodynamic modeling indicated the potential for significant reduction of PuO2(am) to relatively soluble Pu(III). Introduction of Eu(III) or Nd(III) to the suspensions as competitive cations to displace possible sorbed Pu(III) resulted in the release of significant concentrations of aqueous Pu. However, the similarity of aqueous Pu concentrations that resulted from the introduction of Eu(III)/Nd(III) to suspensions with and without magnetite indicated that the Pu was displaced from the PuO2(am), not from magnetite. The fact that soluble forms of Pu can be displaced from the surface of PuO2(am) represents a potential, but previously unidentified, source of Pu to aqueous solution or subsurface groundwaters.},
doi = {10.1021/es3028956},
journal = {Environmental Science & Technology, 46(21):11610-11617},
number = ,
volume = ,
place = {United States},
year = {2012},
month = {11}
}