Synthesis and Characterization of Polyion Complex Micelles with Glycopolymer Shells for Drug Delivery Carriers

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Double hydrophilic diblock copolymers (G 20 A 100 and G 100 A 98 ), composed of non-charged poly(glycosyloxyethyl methacrylate) (PGEMA, G) and cationic poly((3-acrylamidopropyl)trimethylammonium chloride), were synthesized via reversible addition–fragementation chain transfer (RAFT) radical polymerization. Likewise, diblock copolymers (G 20 S 80 and G 100 S 78 ), composed of PGEMA and anionic poly(2-acrylamido-2-methylpropanesulfonate) were synthesized via RAFT. The subscripts in these abbreviations indicate the degree of polymerization (DP) of each block. Polyion complex (PIC) aggregates (G 20 A 100 /G 20 S 80 and G 100 A 98 /G 100 S 78 ) were formed through electrostatic interactions by combining oppositely charged diblock copolymers with matched DPs for charge neutralization. The hydrodynamic radii of the G 20 A 100 /G 20 S 80 and G 100 A 98 /G 100 S 78 PIC aggregates were 77.4 and 26.2 nm, respectively, with zeta potentials close to 0 mV. The G 20 A 100 /G 20 S 80 PIC micelles tend to form intermicellar aggregates, resulting in an increase in the particle size over time. In contrast, G 100 A 98 /G 100 S 78 PIC micelles exhibited colloidal stability with a constant spherical core–shell shape, which was unaffected by time. The morphology and stability of the PIC aggregates depend upon the DP ratio of PGEMA and oppositely charged polyelectrolyte blocks. Both G 20 A 100 /G 20 S 80 and G 100 A 98 /G 100 S 78 PIC aggregates dissociated above 0.8 M NaCl due to the screening effect of NaCl.