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Thermodynamic Analysis of Reaction Equilibria in Ionic and Molecular Liquid Systems by High-Temperature Raman Spectroscopy

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Abstract:

A formalism for correlating relative Raman band intensities with the stoichiometric coefficients, the equilibrium constant, and the thermodynamics of reaction equilibria in solution is derived. The proposed method is used for studying: (1) the thermal dissociation of molten KHSO4 in the temperature range 240–450 °C; (2) the dinuclear complex formation in molten TaCl5–AlCl3 mixtures at temperatures between 125 and 235 °C. The experimental and calculational procedures for exploiting the temperature-dependent Raman band intensities in the molten phase as well as (if applicable) in the vapors thereof are described and used for determining the enthalpy of the equilibria: (1) 2HSO4 (l) ↔ S2O7 2−(l) + H2O(g), ΔH 0=64.9 ± 2.9 kJ mol−1; and (2) 1/2Ta2Cl10(l) + 1/2Al2Cl6(l) ↔ TaAlCl8(l), ΔH 0=−12.1 ± 1.5 kJ mol−1.

Keywords: MOLTEN SALTS; RAMAN BAND INTENSITY CORRELATIONS; RAMAN SPECTROSCOPY; REACTION THERMODYNAMICS

Document Type: Research Article

DOI: http://dx.doi.org/10.1366/000370209789379277

Affiliations: Department of Chemical Engineering, University of Patras and Institute of Chemical Engineering and High Temperature Chemical Processes (FORTH/ICE-HT), GR –26504 Patras, Greece

Publication date: September 1, 2009

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