The interface between the surfaces of clay minerals and other materials (aqueous solution, organic moieties, biomolecules, etc.) is of great importance to many geological, technological and biological processes. The examination of the structure and composition of mineral surfaces is advancing rapidly. However, the crystal structure of a mineral is only part of the information needed to understand the activity of the surface; we still do not fully understand the chemical and physical interactions at the surface or interface. One very powerful methodology for the study of surfaces and interfacial interactions is the determination of the thermodynamic properties of the surface. It became possible in the late 1980s to determine quantitatively the apolar and polar surface-tension components and parameters of liquids and solids (van Oss et al., 1988; van Oss, 1994), and the experimental techniques necessary for obtaining surface free-energy components of minerals, and particularly of colloid-sized minerals, are also a recent development (Costanzo eta!., 1990; van Oss et al., 1990, 1992; Giese et al., 1991).