Abstract
High-temperature gaseous equilibria among the species Th, ThCl, ThCl2, and ThCl3 were studied by mass spectrometry over broad temperature ranges; both enthalpy and entropy data were derived by the second law procedure. In addition, the sublimation of ThCl4 was studied by the torsion-effusion method and the thermodynamics of the gaseous tetrachloride were evaluated. Individual bond dissociation energies in ThCl4 fall within the range 489–545 kJ mol−1, and vary with ligand number in a way similar to ThF4. Only ThCl appears to have a significant electronic entropy in the experimental temperature range. For ThCl4 the experimental entropy indicates the likelihood of a regular tetrahedral structure as with ThF4, but unlike the uranium tetrahalides which appear to be distorted tetrahedra. In the mass spectrum of ThCl4, the fragment ions ThCl+3, ThCl+2, and ThCl+ show a larger and more nearly correct temperature dependence than the parent ion ThCl+4. Results are compared with those of other thorium and uranium halides.
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