Dissolution of uranium dioxide in nitric acid media: what do we know?

Philippe Marc (1) , Alastair Magnaldo (1) , Aimé Vaudano (1) , Thibaud Delahaye (1) , Éric Schaer (2)

1 DMRC - Département de recherche sur les procédés pour la mine et le recyclage du combustible
2 LRGP - Laboratoire Réactions et Génie des Procédés

This article draws a state of knowledge of the dissolution of uranium dioxide in nitric acid media. The chemistry of the reaction is first investigated, and two reactions appear as most suitable to describe the mechanism, leading to the formation of monoxide and dioxide nitrogen as reaction by-products, while the oxidation mechanism is shown to happen before solubilization. The solid aspect of the reaction is also investigated: manufacturing conditions have an impact on dissolution kinetics, and the non-uniform attack at the surface of the solid results in the appearing of pits and cracks. Last, the existence of an autocatalytic mechanism is questionned. The second part of this article presents a compilation of the impacts of several physico-chemical parameters on the dissolution rates. Even though these measurements have been undertaken under a broad variety of conditions, and that the rate determining step of the reaction is usually not specified, general trends are drawn from these results. Finally, it appears that several key points of knowledge still have to be clarified concerning the dissolution of uranium dioxide in nitric acid media, and that the macroscopic scale which has been used in most studies is probably not suitable.

Domains: Chemical Sciences; Chemical engineering; Chemical Sciences; Radiochemistry; Chemical Sciences; Theoretical and/or physical chemistry; Chemical Sciences; Catalysis

Philippe Marc, Alastair Magnaldo, Aimé Vaudano, Thibaud Delahaye, Éric Schaer. Dissolution of uranium dioxide in nitric acid media: what do we know?. EPJ N - Nuclear Sciences & Technologies, 2017, 3 (13), pp.1-13. ⟨10.1051/epjn/2017005⟩. ⟨cea-01516479⟩