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; Blanco, Oliver Dieste; Shuh, David K.; Tyliszcak, Tolek; Venault, Laurent; Moisy, Philippe; Nikitenko, Sergey I.

doi:10.1038/srep43514

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

Journal Article · Fri Mar 03 00:00:00 EST 2017 · Scientific Reports

DOI:https://doi.org/10.1038/srep43514· OSTI ID:1409429

Dalodière, Elodie ^[1]; Virot, Matthieu ^[1]; Morosini, Vincent ^[1]; Chave, Tony ^[1]; Dumas, Thomas ^[2]; Hennig, Christoph ^[3]; Wiss, Thierry ^[4]; Blanco, Oliver Dieste ^[4]; Shuh, David K. ^[5]; Tyliszcak, Tolek ^[5]; Venault, Laurent ^[2]; Moisy, Philippe ^[2]; Nikitenko, Sergey I. ^[1]

Institut de Chimie Separative de Marcoule, Bagnols-sur-Ceze (France)
CEA/DEN/MAR/DRCP, Bagnols-sur-Ceze (France)
Helmholtz-Zentrum Dresden-Rossendorf, Dresden (Germany)
Joint Research Centre (JRC), Institute for Transuranium Elements (ITU), Karlsruhe (Germany)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

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.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231

OSTI ID:: 1409429

Alternate ID(s):: OSTI ID: 22962518

Journal Information:: Scientific Reports, Journal Name: Scientific Reports Vol. 7; ISSN 2045-2322

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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A Novel Metastable Pentavalent Plutonium Solid Phase on the Pathway from Aqueous Plutonium(VI) to PuO ₂ Nanoparticles Kvashnina, Kristina O.; Romanchuk, Anna Yu.; Pidchenko, Ivan Angewandte Chemie International Edition, Vol. 58, Issue 49 https://doi.org/10.1002/anie.201911637	journal	December 2019
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Extension of the Plutonium Oxide Nanocluster Family to Include {Pu ₁₆ } and {Pu ₂₂ } Sigmon, Ginger E.; Hixon, Amy E. Chemistry - A European Journal, Vol. 25, Issue 10 https://doi.org/10.1002/chem.201805605	journal	January 2019
Redox-mediated formation of plutonium oxide nanoparticles Romanchuk, Anna Yu.; Plakhova, Tatiana V.; Egorov, Alexander V. Dalton Transactions, Vol. 47, Issue 32 https://doi.org/10.1039/c8dt02396d	journal	January 2018
Probing the local structure of nanoscale actinide oxides: a comparison between PuO ₂ and ThO ₂ nanoparticles rules out PuO _2+x hypothesis Bonato, Laura; Virot, Matthieu; Dumas, Thomas Nanoscale Advances, Vol. 2, Issue 1 https://doi.org/10.1039/c9na00662a	journal	January 2020
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