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The solubility of Th(IV) hydrous oxide in concentrated NaCl and MgCl[sub 2] solutions

Novak, C.F.

The solubility of Th(IV) hydrous oxide was studied in concentrated 4m and 6m NaCl solutions as well as in MgCl[sub 2] solutions ranging in concentration from 1m to 3m over a broad range of hydrogen ion concentrations. The observed solubilities in all solutions showed the same trend as observed previously of higher solubilities at early equilibration times, usually 7 to 8 days, followed by decreases in solubility with time as the precipitates aged. The trend of decreasing solubility with time was more pronounced in NaCl solutions than in MgCl[sub 2] solutions. The observed ThO[sub 2](am) solubilities in concentrated NaCl solutions (i.e., 4m and 6m) were lower than previously reported solubilities in more dilute NaCl solutions (i.e., < 3M NaCl). The results in MgCl[sub 2] were similar in all solutions regardless of the MgCl[sub 2] concentration. Current thermodynamic models for the solubility of hydrous thorium, oxide in chloride solutions, which primarily describe only aqueous Th[sup 4+]-Cl[sup -] ion-interactions, predicted higher solubilities than observed in 4 and 6m NaCl as well as in all MgCl[sub 2] solutions. An improved aqueous thermodynamic model, which includes ion-interaction parameters for like charged species, is proposed to explain these results.