Interactions between chlorpheniramine (CP), an antihistamine drug used to treat allergy, and 2:1 phyliosilicates were studied under batch kinetic and different solution conditions to investigate the effect of charge density of the substrates on CP removal from solution. The CP removal by Na-montmorillonite was instantaneous, with a very large rate constant and a fast rate, reaching a capacity of 0.64 mmol/g, compared to its cation exchange capacity of 0.85 mmol(c)/g. In contrast, CP removal by talc was 10 times lower at 0.06 mmol/g. Stoichiometric desorption of exchangeable cations accompanying CP removal by Na-montmorillonite confirmed cation exchange as the dominant interaction mechanism. Solution pH had a minimal effect on CP removal by Na-montmorillonite until pH 11. On the contrary, a slight increase in CP removal by talc was observed as the solution pH increased, due to increased negative charges on the pH-dependent surfaces of talc. Interactions between CP and Na-montmorillonite occurred on both external and interlayer sites, resulting in a d-spacing expansion from 12.5 angstrom to 15.2 angstrom. In contrast, interactions between CP and talc were only limited to the external surfaces. It was the charge density that ultimately controlled the amount of CP removal by 2:1 phyllosilicates. Thus, montmorillonite offers a superior option for the removal of cationic drugs from aqueous solution. (C) 2012 Elsevier Inc. All rights reserved.