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Based on a mathematical consistency condition, new relations among the concentration fluctuation integrals in mixtures are derived. These relations indicate that for a binary mixture only one of the fluctuation integrals is independent. A closure procedure is proposed to relate G11 and G22 to G 12 in order to obtain analytic expressions for fluctuation integrals and the related direct correlation integrals. New experimental fluctuation integral data for binary mixtures of tetra­ chloromethane with six organic fluids (methanol, ethanol, propanol, n-butanol, tetrahydrofuran, and 1,4-dioxane ), water + methanol at different temperatures and water + ethanol at different temperatures are reported. The new data and the binary data of water with ten organic fluids (acetone, acetonitri\e, 2-aminoethanol, dimethylsulfoxide, methanol, ethanol, propanol, tert-butanol, tetrahydrofuran, and 1,4-dioxane) are used to test the validity of the proposed theory. Considering the limitations of the closure procedure and the accuracy of the experimental data it is shown that the theory is in agreement with the data.

Relations Among Concentration Fluctuation Integrals in Mixtures (Theory and Experiments)