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On the Regular Behavior of a Binary Mixture of Ionic Liquids.

Binary mixtures of the ionic liquids 1-ethyl-3-methylimidazolium dicyanamide and tributyl(methyl)ammonium dicyanamide, [C2C1im]x[N4441](1-x)[N(CN)2], are studied by means of their excess properties (enthalpy and volume), their viscosity and their Raman spectra. The mixtures exhibit positive values of excess volume VE and excess enthalpy HE. The plot of the logarithm of viscosity as a function of composition is consistent with the finding HE > 0. The excess thermodynamic properties of the ionic liquid mixtures are compared with well-known results for binary mixtures of (high temperature) molten salts. The asymmetry of the curve HE vs. composition is reproduced by considering the volumetric fraction of the [C2C1im]x[N4441](1-x)[N(CN)2] mixtures according to basic results of the theory of regular solutions. The anion totally symmetric stretching mode vs(CN) was used to probe the local environment around the anion in a Raman spectroscopy investigation of the [C2C1im]x[N4441](1-x)[N(CN)2] mixtures as a function of the composition. The Raman band shape (peak frequency and bandwidth) of the s(CN) mode changes as expected from the fluctuation of concentration around the probe oscillator according to models for vibrational spectroscopy of liquid mixtures. This thermodynamic and spectroscopic study lead to the classification of the [C2C1im]x[N4441](1-x)[N(CN)2] mixture as a regular solution. The application of the regular solution equation for HE to others ionic liquids binary mixtures is discussed.