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Structural contributions to AS (hence to S E ) reflect primarily the relative strengths of competing intermolecular attractions Consider the mixing of a nonassociating polar species (eg, acetone) with a nonpolar species (eg, n-hexane) Energetically, the net result of the mixing process is determined primarily by the energy associated with disruption of dipoleldipole interactions, as discussed earlier with respect to H E for NANP mixtures With respect to entropy, this is a structure-breaking process wherein molecular aggregates promoted by a strong dipoleldipole interaction are broken up by mixing Consider instead the mixing of two nonassociating polar species, one a hydrogen donor and the other a hydrogen acceptor [eg, chloroform/acetone,Fig 1 14(c)]Energetically, the net result of the mixing process is determined primarily by the energy associated with formation of a solvation complex, as discussed earlier regarding H E for solvating NA/NA mixtures This is a structure-making process, wherein molecular aggregates promoted by a strong quasichemical interaction are formed on mixing Structure breaking implies a positive contribution to S E (AS > a s i d ) , and structure making a negative contribution to S" (AS < n s i d ) When used in conjunction with sizelshape arguments, these simple notions help to explain observed signs for s E By way of example, we consider again binary liquid mixtures of the kinds discussed in Sec 166

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In the absence of significant sizelshape effects, S E is usually positive, owing to the relative weakness of unlike vs like intermolecular attractions Thus structure breaking on mixing is a stronger effect than structure making However, the enthalpy contribution to GE often dominates, and Region I behavior obtains For mixtures of species of significantly different size (eg, n-hexaneln-hexadecane), positive sizeishape contributions can reinforce structural effects, producing values of sE large enough for entropy to dominate; G E is then negative and Region VI behavior is observed o N A M Mixtures f As already noted, the mixing process here primarily involves structure breaking (positive contributions to S E) Sizelshape effects can have an augmenting influence to produce substantial positive s" However, H E often is also large, and enthalpy usually dominates (Region I) o AS/NP Mixtures f Mixing nominally promotes a structure-breaking disruption of hydrogen-bonded complexes of the associating species However, the persistence of these complexes in solution up to rather high dilution can greatly reduce this positive contribution to sE, leading to negative values of S E over much of the composition range This effect is observed for mixtures of strong associators (eg, alcohols and carboxylic acids) with hydrocarbons An example is the ethanolln-heptane system of Fig 114(d), which shows Region I1 behavior

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As noted in earlier discussion, this is predominately a structure-making situation, and S E is negative However, H E is also negative (and large), whence enthalpy usually dominates, making G E negative (Region IV)

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The complexities discussed with respect to H~ also apply to s E ; structure-breaking and structure-making effects compete to provide a variety of sign combinations and a range of magnitudes for S E

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