Experimental and modelling study of ruthenium extraction with tri-n-butylphosphate in the purex process

P. Moeyaert (1, 2) , M. Miguirditchian (1, 2) , M. Masson (2) , B. Dinh (2) , X. Heres (2) , S. de Sio (3) , C. Sorel (1, 2)

1 DMRC - Département de recherche sur les procédés pour la mine et le recyclage du combustible
2 CEA-DES (ex-DEN) - CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire)
3 AREVA

Ruthenium extraction by tri-n-butylphosphate (TBP) from nitric acid was studied and modelled in the conditions of the PUREX process. Experimental distribution ratios obtained for water, nitric acid and ruthenium were described with a physicochemical model based on the application of the mass action law on each extraction equilibrium and by taking into account deviations from thermodynamic ideal behaviour both in aqueous and organic phase using Mikulin and Sergievskii-Dannus equations. The best agreement between experimental and calculated ruthenium extraction isotherms was obtained by considering the formation of two complexes TBP$_2$RuNO (NO$_3$)$_3$(H$_2$O)$_2$ and TBP$_3$RuNO (NO$_3$)$_3$(H$_2$O)$_2$ ̅̅in organic phase. This model was implemented in the CEA-AREVA PAREX process simulation code and used to simulate ruthenium behaviour in a counter-current PUREX hot test performed in mixer-settlers.

Mots clés: Ruthenium; Nitric acid; Uranium; TBP; Solvent extraction; Modelling

Domaines: Physique Nucléaire Théorique [nucl-th]; Physique Nucléaire Expérimentale [nucl-ex]

P. Moeyaert, M. Miguirditchian, M. Masson, B. Dinh, X. Heres, et al.. Experimental and modelling study of ruthenium extraction with tri-n-butylphosphate in the purex process. Chemical Engineering Science, 2017, 158, pp.580-586. ⟨10.1016/j.ces.2016.10.035⟩. ⟨cea-02388818⟩