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The adsorption ability of natural clay minerals and zeolites is a structurally caused distinguished feature, which determines their physical-chemical properties and almost each area of application. The type of surface active sites responsible for adsorption behavior differs for various structural types of aluminosilicates and varies under modifying agents. The present chapter illustrates the effect of the acid and base modification of natural aluminosilicates on their adsorption behavior in respect to a number of pollutants present in aqueous media. For this, the change of adsorption-structural characteristics of natural clay samples containing representatives of the main groups of clay minerals under activation is considered. Further, the chapter focuses on characterization of surface active sites by means of a new method of a catalytic conversion of 2-methylbut-3-yn-2-ol. The presence of both acid and basic sites on the aluminosilicates surface as well as variations of surface acidity and basicity for different structural types of aluminosilicates under varying conditions of modification is discussed. The third highlight of the chapter encompasses adsorption processes taking place in aqueous solutions of formaldehyde, acetic acid, and ammonium chloride on the surface of natural and activated aluminosilicates. The activating effect of a number of inorganic acids and bases on adsorption equilibrium is compared. The considered mechanism of the adsorption of electrolytes and polar molecules from aqueous media may comprise hydrogen bonding, chemisorptions, or ion-exchange reactions.

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