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a b s t r a c tThe capacities of natural and modified Brazilian bentonite samples as adsorbents to remove hexavalent metal chromium were investigated under several conditions in batch and column methods. The raw material, Ca-bentonite, was modified by anchorament of 3-aminopropyltrietoxisilane (APS) and 3,2-aminoethylaminopropyltrimetoxisilane (AEAPS) in the surface of bentonite sample. This type of new occurrence of bentonite is suitable as a raw material for adsorption process. Adsorption behavior of three bentonite types was strongly depending on pH of adsorbate solution, contact time adsorbent/adsorbate, and initial concentration of Cr(VI). The results were confirmed by column method and reveals that the adsorption process of materials accorded by the Redlich-Peterson, Sips, Dubinin-Radushkevich, and Langmuir isotherm models. The exothermic enthalpic values reflected a favorable energetic process for chromium ions anchored in the material surfaces. The negative Gibbs free energy results supported the spontaneity of three adsorption reactions with Cr(VI) ions.