Natural montmorillonite (M) and synthetic kanemite (K) have been functionalized with 1,4-bis(3-aminopropyl)piperazine reacted with methylacrylate to yield new inorganic-organic chelating materials. The original and modified materials were characterized by X-ray diffractometry, textural analysis, SEM and nuclear magnetic nuclei of carbon-13 and silicon-29. The chemically modified clay samples (M-APPMA and K-APPMA) showed modification of its physical-chemical properties including: specific area 45.0 m(2) g(-1) (M) to 978.8 m(2) g(-1) (M-APPMA) and 23.5 m(2) g(-1) (K) to 898.9 m(2) g(-1) (K-APPMA). The ability of these materials to remove thorium(IV), uranyl(VI) and europium(III) from aqueous solution was followed by a series of adsorption isotherms, which were fitted to non-linear Sips adsorption isotherm model. To achieve the best adsorption conditions the influence of pH and variation of metal concentration were investigated. The energetic effects (Delta H-int degrees, Delta(int)G degrees and Delta S-int degrees) caused by metal ions adsorption were determined through calorimetric titrations. (C) 2009 Published by Elsevier B.V.