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Abstract:
New Surfactant PolyIon Complex (SPIC) micelles were assembled by electrostatic complexation of an antibacterial cationic surfactant, cetylpyridinium chloride (CPC), and a double hydrophilic block copolymer (DHBC) containing a neutral comb block of poly(oligo(ethylene glycol)) methyl ether acrylate (PEOGA) and a weak polyacid block of poly(acrylic acid) (PAA). The corresponding SPIC micelles, with a CPC/PAA core and a PEOGA corona, were successfully used as structure directing and functionalizing agents in a soft and sustainable sol-gel strategy, yielding hybrid mesoporous silica (MS) materials with a monomodal pore size distribution centred at 2.8 nm. The influence of synthesis parameters, including the pH, concentrations and ratios of components, was systematically investigated. The obtained hybrid MS materials were intrinsically functional, with PEOGA blocks anchored in silica walls via H-bonding, while weak polyacid blocks, complexed with CPC, were confined within the mesopores. The response of the materials to pH changes (pH 7.4, 4.2 and 3) indicated remarkable stability of the anchored DHBC, while CPC was selectively released under the acidic conditions typical of orodental biofilm microenvironments. This result is noteworthy, since the release of encapsulated amphiphilic drugs into water is less favorable than that of hydrophilic drugs. Owing to the control of their pore and functionality properties, ordered hybrid silica materials templated and functionalized with SPIC systems will be materials of choice for developing pH-responsive biomedical devices using wet processing techniques

Keywords:
Double hydrophilic block copolymer, Cooperative self-assembly, Surfactant-polyion complex micelle, Stimuli-responsive nanomaterials, Sustainable, Sol-gel synthesis