The intercalation of a cubical octamer derived from the controlled hydrolysis of 3-aminopropyltriethoxysilane with smectite clays has been examined. The organosilicon cubanes are adsorbed in an amount that exceeds the cation exchange capacity of the mineral. The excess quantity is incorporated in the form of physically adsorbed ion pairs. The results suggest that the physically adsorbed ionpaired cubic units, participate in alkylation reactions affording the corresponding tetraalkylammonium derivatives under triphase conditions. The alkylated products were studied by chemical analysis, X-ray diffraction and FT-infrared spectroscopy.