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Title: Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids

Abstract

Fundamental knowledge on intrinsic plutonium colloids is important for the prediction of plutonium behaviour in the geosphere and in engineered systems. The first synthetic route to obtain salt-free intrinsic plutonium colloids by ultrasonic treatment of PuO2 suspensions in pure water is reported. Kinetics showed that both chemical and mechanical effects of ultrasound contribute to the mechanism of Pu colloid formation. In the first stage, fragmentation of initial PuO2 particles provides larger surface contact between cavitation bubbles and solids. Furthermore, hydrogen formed during sonochemical water splitting enables reduction of Pu(IV) to more soluble Pu(III), which then re-oxidizes yielding Pu(IV) colloid. A comparative study of nanostructured PuO2 and Pu colloids produced by sonochemical and hydrolytic methods, has been conducted using HRTEM, Pu LIII-edge XAS, and O K-edge NEXAFS/STXM. Characterization of Pu colloids revealed a correlation between the number of Pu-O and Pu-Pu contacts and the atomic surface-to-volume ratio of the PuO2 nanoparticles. NEXAFS indicated that oxygen state in hydrolytic Pu colloid is influenced by hydrolysed Pu(IV) species to a greater extent than in sonochemical PuO2 nanoparticles. In general, hydrolytic and sonochemical Pu colloids can be described as core-shell nanoparticles composed of quasi-stoichiometric PuO2 cores and hydrolyzed Pu(IV) moieties at the surface shell.

Authors:
 [1];  [1];  [1];  [1];  [2];  [3];  [4];  [4];  [5];  [5];  [2];  [2];  [1]
+ Show Author Affiliations
  1. Institut de Chimie Separative de Marcoule, Bagnols-sur-Ceze (France)
  2. CEA/DEN/MAR/DRCP, Bagnols-sur-Ceze (France)
  3. Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany)
  4. Joint Research Centre (JRC), Institute for Transuranium Elements (ITU), Karlsruhe (Germany)
  5. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1409429
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Dalodière, Elodie, Virot, Matthieu, Morosini, Vincent, Chave, Tony, Dumas, Thomas, Hennig, Christoph, Wiss, Thierry, Blanco, Oliver Dieste, Shuh, David K., Tyliszcak, Tolek, Venault, Laurent, Moisy, Philippe, and Nikitenko, Sergey I. Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids. United States: N. p., 2017. Web. doi:10.1038/srep43514.
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Dalodière, Elodie, Virot, Matthieu, Morosini, Vincent, Chave, Tony, Dumas, Thomas, Hennig, Christoph, Wiss, Thierry, Blanco, Oliver Dieste, Shuh, David K., Tyliszcak, Tolek, Venault, Laurent, Moisy, Philippe, & Nikitenko, Sergey I. Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids. United States. https://doi.org/10.1038/srep43514
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Dalodière, Elodie, Virot, Matthieu, Morosini, Vincent, Chave, Tony, Dumas, Thomas, Hennig, Christoph, Wiss, Thierry, Blanco, Oliver Dieste, Shuh, David K., Tyliszcak, Tolek, Venault, Laurent, Moisy, Philippe, and Nikitenko, Sergey I. Fri . "Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids". United States. https://doi.org/10.1038/srep43514. https://www.osti.gov/servlets/purl/1409429.
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@article{osti_1409429,
title = {Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids},
author = {Dalodière, Elodie and Virot, Matthieu and Morosini, Vincent and Chave, Tony and Dumas, Thomas and Hennig, Christoph and Wiss, Thierry and Blanco, Oliver Dieste and Shuh, David K. and Tyliszcak, Tolek and Venault, Laurent and Moisy, Philippe and Nikitenko, Sergey I.},
abstractNote = {Fundamental knowledge on intrinsic plutonium colloids is important for the prediction of plutonium behaviour in the geosphere and in engineered systems. The first synthetic route to obtain salt-free intrinsic plutonium colloids by ultrasonic treatment of PuO2 suspensions in pure water is reported. Kinetics showed that both chemical and mechanical effects of ultrasound contribute to the mechanism of Pu colloid formation. In the first stage, fragmentation of initial PuO2 particles provides larger surface contact between cavitation bubbles and solids. Furthermore, hydrogen formed during sonochemical water splitting enables reduction of Pu(IV) to more soluble Pu(III), which then re-oxidizes yielding Pu(IV) colloid. A comparative study of nanostructured PuO2 and Pu colloids produced by sonochemical and hydrolytic methods, has been conducted using HRTEM, Pu LIII-edge XAS, and O K-edge NEXAFS/STXM. Characterization of Pu colloids revealed a correlation between the number of Pu-O and Pu-Pu contacts and the atomic surface-to-volume ratio of the PuO2 nanoparticles. NEXAFS indicated that oxygen state in hydrolytic Pu colloid is influenced by hydrolysed Pu(IV) species to a greater extent than in sonochemical PuO2 nanoparticles. In general, hydrolytic and sonochemical Pu colloids can be described as core-shell nanoparticles composed of quasi-stoichiometric PuO2 cores and hydrolyzed Pu(IV) moieties at the surface shell.},
doi = {10.1038/srep43514},
journal = {Scientific Reports},
number = ,
volume = 7,
place = {United States},
year = {Fri Mar 03 00:00:00 EST 2017},
month = {Fri Mar 03 00:00:00 EST 2017}
}
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    A Novel Metastable Pentavalent Plutonium Solid Phase on the Pathway from Aqueous Plutonium(VI) to PuO 2 Nanoparticles
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    • Kvashnina, Kristina O.; Romanchuk, Anna Yu.; Pidchenko, Ivan
    • Angewandte Chemie International Edition, Vol. 58, Issue 49
    • DOI: 10.1002/anie.201911637
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