Chitosan beads were cross‐linked with glutaraldehyde (GA) and epichlorohydrin (EP), respectively, at variable composition. The general features of the adsorptive and textural properties of the bead systems were characterized using p‐nitrophenolate (PNP) at pH 8.5. As well, a systematic adsorption study of phosphate dianion (phosphate (
HPO42‐) species was carried out in aqueous solution at pH 8.5 and 295 K. The Sips isotherm model yielded adsorption parameters for the chitosan bead systems: (i) monolayer adsorption capacity (Qm) for PNP ranged from 0.30 to 0.52 mmol g−1 and (ii) Qm values for the bead systems with
HPO42‐ ranged from 22.4–52.1 mg g−1 for these conditions. GA cross‐linked beads reveal greater Qm values for PNP while EP cross‐linked beads showed greater Qm values for
HPO42‐, in accordance with the surface chemistry and the materials design described herein. The EP cross‐linked beads show favorable adsorption–desorption properties and represents a promising tunable adsorbent system for the effective removal of phosphate dianion species in aqueous solution. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 42949.