Abstract
The electromotive force and its temperature-dependence of fused salts of the ThCl 4 –NaCl system were measured with a Th(s)/ThCl 4 –NaCl(l)/Cl 2 (g) cell using highly purified ThCl 4 (ThCl 4 0.22–0.70 mole fraction, 600°–750°C). To discuss the formation and existence of complex ion in the melts, the equation of excess stability d\bar F 1 E /d(1- N 1 ) 2 , where N 1 is the mole fraction of ThCl 4 and \bar F 1 E the excess partial molar free energy of ThCl 4 , derived by Darken was adopted. Curves of the excess stability plotted against N 1 show a maximum at around N 1 =0.35 corresponding to the congruently melting compound Na 2 ThCl 6 . Meanwhile, plots of the equivalent conductivity and the isotherms, calculated from the previously reported values against N 1 revealed a large negative deviation from the additivity at N 1 =0.33(550°C–750°C). From these both results the existence of the anionic complex ion [ThCl 6 ] 2- in the fused state was inferred.
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