Issue 21, 2016

Ultrasound-assisted reductive dissolution of CeO2 and PuO2 in the presence of Ti particles

Abstract

PuO2 is considered an important material for current and future nuclear fuel; however it is a very refractive compound towards dissolution. Among other techniques, its reprocessing can be performed via complexing dissolution in concentrated and boiling nitric acid containing hydrofluoric acid, or via oxidant dissolution in the presence of reagents with redox couples having high potentials such as Ce(IV)/Ce(III), or Ag(II)/Ag(I). Reductive dissolution can be performed under softer conditions and is considered an alternative to these methods which may suffer from several drawbacks (corrosion, effluent management, compatibility with nuclear waste disposal, etc.). In this study, a sonochemical and reductive approach is investigated for PuO2 dissolution under relatively mild conditions. At the first stage, the experiments are performed with CeO2 as an inactive surrogate for PuO2. The quantitative dissolution of both oxides can be achieved under ultrasound (20 kHz, 0.35–0.70 W mL−1) in 0.5 M HNO3/0.1 M [N2H5NO3]/2 M HCOOH sparged with Ar at 33–35 °C in the presence of Ti particles as a generating source of reductive species. Ultrasound enables the depassivation of the Ti surface (usually strongly passivated in nitric solutions) through acoustic cavitation which then allows further generation of the intermediate Ti(III) reductive species. Dissolution rates and yields can be further increased with the injection of dilute fluoride aliquots (NH4F or HF) in the sonicated solution to favor Ti chemical depassivation. The rapid and complete dissolution of PuO2 under selected conditions is accompanied by Pu(III) accumulation in solution.

Graphical abstract: Ultrasound-assisted reductive dissolution of CeO2 and PuO2 in the presence of Ti particles

Supplementary files

Article information

Article type
Paper
Submitted
18 Dec 2015
Accepted
17 Apr 2016
First published
20 Apr 2016

Dalton Trans., 2016,45, 8802-8815

Ultrasound-assisted reductive dissolution of CeO2 and PuO2 in the presence of Ti particles

X. Beaudoux, M. Virot, T. Chave, G. Leturcq, G. Jouan, L. Venault, P. Moisy and S. I. Nikitenko, Dalton Trans., 2016, 45, 8802 DOI: 10.1039/C5DT04931H

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