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Grenthe, I.; Robouch, P.; Vitorge, P.
CEA Centre d'Etudes Nucleaires de Fontenay-aux-Roses, 92 (France). Inst. de Recherche Technologique et de Developpement Industriel (IRDI)1985
CEA Centre d'Etudes Nucleaires de Fontenay-aux-Roses, 92 (France). Inst. de Recherche Technologique et de Developpement Industriel (IRDI)1985
AbstractAbstract
[en] By using spectrophotometric and potentiometric methods it is shown that, in media of high ionic strength (NaClO4 3M) and total concentrations of hexavalent actinoids higher than 10-3M, trimers are formed. The equilibrium constants for the reactions 3MO2(CO3)34- reversible (MO2)3(CO3)66- + 3 CO32- are log K (U) = -11,3; log K (Np) = -10,1 and log K (Pu) = -7,4. It is demonstrated that one of the cations of the trimer can be exchanged with another actinoid cation: the equilibrium constants for the reactions 2UO2 (CO3)34- + MO2 (CO34- reversible (UO2)2 MO2 (CO3)66- + 3CO33- are log K = -11,3; -10,0 and -8,8 respectively for M: U, Np, Pu. Then, polynuclear complexes can be efficient solution ''carriers'' for other hexavalent actinides in a waste disposal. Some properties of the solid phases MO2CO3(s) are discussed. Experimental studies of chemical equilibria of americium (III, IV) are reviewed: in carbonate media Am(III) species are Am CO3+, Am (CO3)2- Am (CO3)33-, (Am2 CO3)sub(s) and (NaAm(CO3)2)sub(s); for Am(IV), log B5 approximately equal to 40. In NaClO4 (3M) medium solubility measurements of Np(V) show that logβ1 = 5,09, logβ2 = 8,15, logβ3 = 10,46, log Ks(Na Np O2 CO3) = 10,56 and log Ks (Na3 NpO2(CO3)2) = 12,44; ionic strength corrections are proposed
Source
Sep 1985; 8 p; Actinides 85 conference; Aix-en-Provence (France); 2-6 Sep 1985
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