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Herein, a novel method for molecularly imprinted polymers (MIPs) using methacrylic acid functionalized beta-cyclodextrin (MAA-&#946;-CD) monomer is presented, which was designed as a potential water-compatible composite for the controlled release of atropine (ATP). The molecularly imprinted microspheres with pH-sensitive characteristics were fabricated using thermally-initiated precipitation polymerization, employing ATP as a template molecule. The effects of different compounds and concentrations of cross-linking agents were systematically investigated. Uniform microspheres were obtained when the ratio between ATP, MAA-&#946;-CD, and trimethylolpropane trimethacrylate (TRIM) was 1:4:20 (mol/mol/mol) in polymerization system. The ATP loading equilibrium data was best suited to the Freundlich and Langmuir isotherm models. The <i>in vitro</i> drug release study was assessed under simulated oral administration conditions (pH 1.5 and 7.4). The potential usefulness of MIPs as drug delivery devices are much better than non-molecularly imprinted polymers (NIPs). The study shows that the prepared polymers are a pH stimuli-responsive system, which controlled the release of ATP, indicating the potential applications in the field of drug delivery.