A quantity termed the total surface segregation is discussed and evaluated as a measure of relative adsorption at the gas-liquid interface of binary liquid mixtures. Its calculation from the surface tension and nonideality of the liquid mixture is detailed, and results are presented for 17 systems covering the recognized classes of liquid mixtures. The results for argon + krypton, in particular, are compared with theoretical calculations based on the density functional treatment of Telo da Gama and Evans which yields the local surface segregation whose integral through the interface is a close approximation to the total surface segregation. The absolute magnitude, composition dependence, relation to surface azeotropy (aneotropy) and bulk azeotropy, and proximity to a consolute point of the total surface segregation are explored. Useful relationships with the known underlying intermolecular forces are presented which confirm broadly the utility of the total surface segregation for the purpose of representing adsorption at the gas-liquid interface of mixtures.
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