Using aminoglycoside antibiotics as drug models, it was shown that electrostatic complexes between hydrophilic drugs and oppositely charged double-hydrophilic block copolymers can form ordered mesophases. This phase behavior was evidenced by using poly(acrylic acid)-block-poly(ethylene oxide) block copolymers in the presence of silica precursors, and this allowed preparing drug-loaded mesoporous silica directly from the drug-polymer complexes. The novel synthetic strategy of the hybrid materials is highly efficient, avoiding waste and multistep processes; it also ensures optimal drug loading and provides pH-dependence of the drug release from the materials.

Ordered mesoporous silica materials were prepared under different pH conditions by using a silicon alkoxide as a silica source and polyion complex (PIC) micelles as the structure-directing agents. PIC micelles were formed by complexation between a weak polyacid-containing double-hydrophilic block copolymer, poly(ethylene oxide)-b-poly(acrylic acid) (PEO-b-PAA), and a weak polybase, oligochitosan-type polyamine. As both the micellization process and the rate of silica condensation are highly dependent on pH, the properties of silica mesostructures can be modulated by changing the pH of the reaction medium. Varying the materials synthesis pH from 4.5 to 7.9 led to 2D-hexagonal, wormlike or lamellar mesostructures, with a varying degree of order. The chemical composition of the as-synthesized hybrid organic/inorganic materials was also found to vary with pH. The structure variations were discussed based on the extent of electrostatic complexing bonds between acrylate and amino functions and on the silica condensation rate as a function of pH.

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