Journal
POLYMER CHEMISTRY
Volume 8, Issue 38, Pages 5962-5971Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c7py01306j
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Funding
- EPSRC [EP/L024160, EP/K030949]
- ERC Advanced Investigator grant [PISA 320372]
- EPSRC [EP/J007846/1, EP/K030949/1] Funding Source: UKRI
- Engineering and Physical Sciences Research Council [EP/J007846/1, EP/K030949/1] Funding Source: researchfish
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The recent development of polymerization-induced self-assembly (PISA) has facilitated the rational synthesis of a range of diblock copolymer worms, which hitherto could only be prepared via traditional postpolymerization processing in dilute solution. Herein we explore a new synthetic route to aqueous dispersions of cationic disulfide-functionalized worm gels. This is achieved via the PISA synthesis of poly[(glycerol monomethacrylate-stat-glycidyl methacrylate)]-block-poly(2-hydroxypropyl methacrylate) (P(GMAstat- GlyMA)-PHPMA) block copolymer worms via reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerization of HPMA. A water-soluble reagent, cystamine, is then reacted with the pendent epoxy groups located within the P(GMA-stat-GlyMA) stabilizer chains to introduce disulfide functionality, while simultaneously conferring cationic character via formation of secondary amine groups. Moreover, systematic variation of the cystamine/epoxy molar ratio enables either chemically cross-linked worm gels or physical (linear) primary amine-functionalized disulfide-based worm gels to be obtained. These new worm gels were characterized using gel permeation chromatography, H-1 NMR spectroscopy, transmission electron microscopy, dynamic light scattering, aqueous electrophoresis and rheology. In principle, such hydrogels may offer enhanced mucoadhesive properties.
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