Abstract

Actinides co-precipitation is currently investigated in order to synthesize solid solutions of actinides mixed oxalates. This paper deals with the thermodynamic and kinetic study of the precipitation of uranium-neodymium oxalate system. Based on an analysis of the theories developed in the literature, a new expression for the determination of the supersaturation ratio for the solid solutions is presented. An experimental study of the nucleation kinetics was performed on the mixed uranium-neodymium oxalates. Homogeneous and heterogeneous primary nucleation laws are obtained using a specific stopped flow apparatus. The experimental results are consistent with the classical behaviour of nucleation phenomena. The values of the kinetic parameters for the solid solution point out that the formation of the uraniumneodymium mixed oxalates is kinetically favoured compared with the simple uranium and neodymium oxalates.

Highlights

  • Current concepts for future nuclear systems aim at improving the fuel cycle with the co-management of actinides in order to enhance the fuel performance and to reduce the proliferation risk

  • This article focuses on the kinetic study in order to determine the primary nucleation rate for the uranium-neodymium oxalate system, which simulates the uranium-actinide system behaviour

  • This paper describes how to obtain new expressions for the determination of equilibrium relation and supersaturation ratio for any solid solution-aqueous solution (SSAS) system

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Summary

Introduction

Current concepts for future nuclear systems aim at improving the fuel cycle with the co-management of actinides in order to enhance the fuel performance and to reduce the proliferation risk. The co-conversion of actinides into oxide can be achieved by different processes such as oxalic co-precipitation, thermal co-denitration or co-gelation. The Oxalic co-precipitation is one investigated way to synthesize solid solutions of actinide mixed oxalates which have to meet strict requirements [2]. To support the process development, the determination of mechanisms and kinetic laws associated with the co-precipitation appears to be a key issue. This article focuses on the kinetic study in order to determine the primary nucleation rate for the uranium-neodymium oxalate system, which simulates the uranium-actinide system behaviour

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