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Functionalization Induced Self-Assembly of Polystyrene/ Kaolinite In situ Nanocomposites into Giant Vesicles.

We report a facile functionalization strategy for fabrication of giant, inorganic-polymer hybrid vesicles by controlled aminosilyl/ vinylsilyl functionalization (AS/VS) of the aluminol layer in kaolinite (Kaol) by intercalation and subsequent polymerization with styrene to in situ nanocomposite (PCN) followed by self-assembly of the delaminated hybrid system. The synergistic effect of AS/VS on functionalization assisted intercalation was established in 1:3AS/VS-Kaol by the greater extent of formation of higher interlayer spacing corresponds to 1.12 nm compared to 1:1AS/VS-Kaol. As the AS:VS has increased, the PCN showed an increase in molecular weight attributed to higher vinyl functionalization of the aluminol layer. 1:3AS/VS-Kaol/PS showed self-assembly in tetrahydrofuran (THF) at 2.5 mg mL-1, into giant vesicular morphology in 2-6 µm diameter with a wall thickness of 300-400 nm. This result is attributed to molecular mass directed bilayer assembly of the delaminated Janus type functionalized-Kaol in polar aprotic solvents by end to end hydrogen bonding involving terminal -OH groups along the wall and lateral -NH2 groups, stabilized by the π-π interactions of the phenyl moiety along the periphery. Rhodamine-loaded vesicles showed a controlled release in buffer solutions of pH, 7.0 or 9.0 attributed to the amino group assisted pore formation. In pH, 4.0, rapid release of the dye has observed attributed to collapse of the vesicle directed by protonation of amino group. This study forms the first report on a novel method for the synthesis of hybrid vesicles by functionalization induced self-assembly of Kaol based in situ PCN for possible applications in the cost-effective controlled delivery of drugs or cosmetics for topical applications.