2017
DOI: 10.1038/srep43514
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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… Show more

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Cited by 45 publications
(101 citation statements)
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“…Figure shows the comparison of the Pu HERFD L 3 edge data recorded for PuO 2 and the intermediate Pu phase during the PuO 2 NPs formation. As discussed previously, the L 3 spectrum of Pu V compounds always shows a very characteristic energy shift towards low energies and a decrease of the L 3 white line intensity compared to Pu IV and Pu VI systems (Figure S3). The chemical shift of the intermediate Pu phase is clearly resolved in the HERFD data reported in Figure and indicates the presence of the Pu V oxidation state, in agreement with the Pu M 4 HERFD results.…”
Section: Figuresupporting
confidence: 73%
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“…Figure shows the comparison of the Pu HERFD L 3 edge data recorded for PuO 2 and the intermediate Pu phase during the PuO 2 NPs formation. As discussed previously, the L 3 spectrum of Pu V compounds always shows a very characteristic energy shift towards low energies and a decrease of the L 3 white line intensity compared to Pu IV and Pu VI systems (Figure S3). The chemical shift of the intermediate Pu phase is clearly resolved in the HERFD data reported in Figure and indicates the presence of the Pu V oxidation state, in agreement with the Pu M 4 HERFD results.…”
Section: Figuresupporting
confidence: 73%
“…In the near‐field conditions of geological repositories of spent nuclear fuel and other radioactive wastes, the formation of intrinsic PuO 2 colloids is a key scenario . Therefore, the characterization of such intrinsic colloidal nanoparticles (NPs) in aqueous solution has recently received much attention . The most debated question is the structural nature of these NPs (crystalline vs. amorphous) as well as the presence of Pu V and other oxidation states in small NPs (<3 nm) .…”
Section: Figurementioning
confidence: 99%
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“…In addition, the central core of each nanocluster exhibits the same fundamental fluorite structure as bulk PuO 2 wherein the eight‐coordinate Pu IV metal centers are connected by μ 4 ‐oxo bridges. The bond lengths reported here are consistent with those reported from X‐ray absorption spectroscopy measurements of plutonium colloids prepared through a variety of synthetic approaches …”
Section: Figurementioning
confidence: 99%
“…A fitting model made of only one oxygen shell either failed to accurately reproduce the spectra or led to unrealistic Debye Waller factors. To overcome this issue with disordered plutonium colloids, several authors have used complementary oxygen shell(s) and adjusted the Pu coordination number to take into account both the average particle size and the short‐range disorder ,,,. The best fit spectra reported in Figure bc were obtained applying the same procedure with two oxygen shells.…”
Section: Figurementioning
confidence: 99%