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On the Solvation Thermodynamics Involving Species with Large Intermolecular Asymmetries: A Rigorous Molecular-Based Approach to Simple Systems with Unconventionally Complex Behaviors.

This work deals with the solvation thermodynamics of systems containing extreme intermolecular interaction asymmetries, such as binary mixtures comprising ideal gas species plus other real species, and analyzes the composition dependence of relevant solvation properties from a rigorous molecular-based theoretical viewpoint. It focuses on the effect of large intermolecular interaction asymmetries, involving simple model species for which we have available rigorous results, to advance our understanding of the true molecular-based origin of their unconventional solvation behavior. This effort involves a statistical mechanics approach to identify the thermodynamic constraints and microstructural manifestation underlying the non-monotonous composition behavior of the species' partial molar properties, as well as to describe formally the explicit link between the intermolecular asymmetries and the observed anomalous behavior. The outcome of the analysis provides sound support to the depiction of the solvation of a weakly-interacting solute in a real solvent, a scenario that facilitates the molecular thermodynamic interpretation of gas solvation characterized by low solubility and thermodynamic stability gaps. Moreover, this work illustrates direct comparisons between real aqueous systems and the ideal gas-aqueous system counterparts to highlight and discuss the usefulness of invoking the ideal gas species as a reference solute to gain understanding of the solvation of real gas species.