Shell-sheddable polymeric assemblies are a type of self-assembled structures formed by amphiphilic block copolymers with cleavable linkages at the junction points. The shell-sheddable self-assemblies have been used as nanocarriers for drugs and inorganic nanoparticles . In this research, synthesis and self-assembly of amphiphilic tadpole-shaped block copolymer with disulfide bonds at the junction points were investigated. Dialkyne-terminated polystyrene (Da-PS) was synthesized by reversible addition-fragmentation chain transfer polymerization and thiol-disulfide exchange reaction. The tadpole-shaped block copolymer was synthesized by bimolecular coupling between azido-terminated PEG and Da-PS. Size exclusion chromatograph , FTIR, 1 H NMR and matrix-assisted laser desorption/ionization time-of-flight (MALDI-TOF) mass analysis results all indicated successful synthesis of the polymer. The tadpole-shaped block copolymer self-assembles into vesicles in aqueous solution. The disulfide bonds at the junction points can be cleaved by a reducing agent, resulting in aggregation of the assemblies.
Linear poly(N-hydroxyethylacrylamide) (PHEAA) is regarded as one of the most promising antifouling materials because of its excellent antifouling properties and good hemocompatibility. However, the antifouling performance of topological PHEAAs remains largely unknown. Herein, the preparation of antifouling surfaces based on a tadpole-shaped PHEAA coating is reported for the first time, and how the tadpole-shaped PHEAA architecture affects antifouling performance is investigated. It is shown that the tadpole-shaped PHEAA-modified surfaces exhibit better antifouling performance than linear copolymer precursor-modified surfaces with identical molar masses and chemical compositions. This may be primarily attributed to the presence of cyclic PHEAA head chain segments in the tadpole-shaped PHEAA copolymer, and the absence of interchain entanglements can facilitate the formation of smoother and densely packed grafts, which result in better antifouling properties.
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