ABSTRACT It is shown that water associated with biopolymers exists in two modified states: stretched water, which has expanded and increased its local partial molar volume, and compacted water which has decreased its local partial molar volume. These populations of water molecules change their local density in order to equilibrate with other populations of molecules of different local chemical potential. Changes of density are accompanied by changes in water-water hydrogen-bond strength and therefore in all the physical and chemical properties of the liquid. Co-existence of assemblies of water molecules with different solvent properties results in asymmetric distributions of solutes. Solutes and water appear to be unable to come to equilibrium. Solutes excluded from stretched water create fresh osmolality gradients which must be compensated for by further expansion of stretched water. Such a gel/solution system approaches an ever-receding free energy minimum. Solutes accumulated into stretched water, on the other hand, if unaccompanied by water, decrease the activity of stretched water, driving it to revert toward its normal structure and solvent properties. In the presence of mixtures of both classes of ions oscillations of water and ion-contents were observed.
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