Article Dans Une Revue Ultrasonics Sonochemistry Année : 2025

Unveiling the Dual Reactivity of Nanoscaled PuO₂ Sonicated in Oxygenated Aqueous Solutions

Résumé

While bulk PuO₂ is known to be highly refractory to dissolution, even under ultrasonic irradiation, this study demonstrates that nanometric PuO₂ samples can exhibit unique reactivity when sonicated under an Ar/(20%)O₂ atmosphere. Interestingly, this reactivity does not appear to be related to nanoparticle size but rather to the preparation method and possibly to the nanoparticle surface state. Sonication of powdered PuO₂ nanoparticles (~5 nm) in pure water was found to be ineffective. In contrast, colloidal PuO₂ nanoparticles (~3 nm) prepared via hydrolysis exhibited markedly different behavior, leading to the accumulation of Pu(VI), with H₂O₂ playing a crucial role in the process. Further investigations identified an intermediate species implicated in the dissolution process, agreeing with a recently described Pu(IV) peroxide compound. Despite the chemical similarity of the PuO₂ nanoparticles, this study highlights their dual reactivity under conditions favoring H₂O₂ formation suggesting an important role of the preparation method. Beyond underscoring the critical role of H₂O₂ in the reactivity of PuO₂ nanoparticles, this study also evidences a potential pathway for their transformation under environmental conditions where radiolysis could generate similar chemical environments.

Dates et versions

cea-05044697 , version 1 (23-04-2025)

Identifiants

Citer

Julien Margate, Matthieu Virot, Thomas Dumas, Simon Bayle, Denis Menut, et al.. Unveiling the Dual Reactivity of Nanoscaled PuO₂ Sonicated in Oxygenated Aqueous Solutions. Ultrasonics Sonochemistry, 2025, 117, pp.107346. ⟨10.1016/j.ultsonch.2025.107346⟩. ⟨cea-05044697⟩
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