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Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids
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 PuO(2) suspensions in pure water is reported....
Autores principales: | , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group
2017
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5335258/ https://www.ncbi.nlm.nih.gov/pubmed/28256635 http://dx.doi.org/10.1038/srep43514 |
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author | Dalodière, Elodie Virot, Matthieu Morosini, Vincent Chave, Tony Dumas, Thomas Hennig, Christoph Wiss, Thierry Dieste Blanco, Oliver Shuh, David K. Tyliszcak, Tolek Venault, Laurent Moisy, Philippe Nikitenko, Sergey I. |
author_facet | Dalodière, Elodie Virot, Matthieu Morosini, Vincent Chave, Tony Dumas, Thomas Hennig, Christoph Wiss, Thierry Dieste Blanco, Oliver Shuh, David K. Tyliszcak, Tolek Venault, Laurent Moisy, Philippe Nikitenko, Sergey I. |
author_sort | Dalodière, Elodie |
collection | PubMed |
description | 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 PuO(2) 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 PuO(2) 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 PuO(2) and Pu colloids produced by sonochemical and hydrolytic methods, has been conducted using HRTEM, Pu L(III)-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 PuO(2) nanoparticles. NEXAFS indicated that oxygen state in hydrolytic Pu colloid is influenced by hydrolysed Pu(IV) species to a greater extent than in sonochemical PuO(2) nanoparticles. In general, hydrolytic and sonochemical Pu colloids can be described as core-shell nanoparticles composed of quasi-stoichiometric PuO(2) cores and hydrolyzed Pu(IV) moieties at the surface shell. |
format | Online Article Text |
id | pubmed-5335258 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2017 |
publisher | Nature Publishing Group |
record_format | MEDLINE/PubMed |
spelling | pubmed-53352582017-03-07 Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids Dalodière, Elodie Virot, Matthieu Morosini, Vincent Chave, Tony Dumas, Thomas Hennig, Christoph Wiss, Thierry Dieste Blanco, Oliver Shuh, David K. Tyliszcak, Tolek Venault, Laurent Moisy, Philippe Nikitenko, Sergey I. Sci Rep Article 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 PuO(2) 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 PuO(2) 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 PuO(2) and Pu colloids produced by sonochemical and hydrolytic methods, has been conducted using HRTEM, Pu L(III)-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 PuO(2) nanoparticles. NEXAFS indicated that oxygen state in hydrolytic Pu colloid is influenced by hydrolysed Pu(IV) species to a greater extent than in sonochemical PuO(2) nanoparticles. In general, hydrolytic and sonochemical Pu colloids can be described as core-shell nanoparticles composed of quasi-stoichiometric PuO(2) cores and hydrolyzed Pu(IV) moieties at the surface shell. Nature Publishing Group 2017-03-03 /pmc/articles/PMC5335258/ /pubmed/28256635 http://dx.doi.org/10.1038/srep43514 Text en Copyright © 2017, The Author(s) http://creativecommons.org/licenses/by/4.0/ This work is licensed under a Creative Commons Attribution 4.0 International License. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in the credit line; if the material is not included under the Creative Commons license, users will need to obtain permission from the license holder to reproduce the material. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ |
spellingShingle | Article Dalodière, Elodie Virot, Matthieu Morosini, Vincent Chave, Tony Dumas, Thomas Hennig, Christoph Wiss, Thierry Dieste Blanco, Oliver 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 |
title | Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids |
title_full | Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids |
title_fullStr | Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids |
title_full_unstemmed | Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids |
title_short | Insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids |
title_sort | insights into the sonochemical synthesis and properties of salt-free intrinsic plutonium colloids |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC5335258/ https://www.ncbi.nlm.nih.gov/pubmed/28256635 http://dx.doi.org/10.1038/srep43514 |
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