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We report synthesis of temperature- and redox-responsive multiblock copolymers by reversible addition-fragmentation chain transfer (RAFT) polymerization. Well-defined α,ω-bis(dithioester)-functionalized poly(N-isopropylacrylamide) (PNIPAM) and poly(2-(dimethylamino) ethyl methacrylate) (PDMAEMA) were prepared using 1,4-bis(thiobenzoylthiomethyl)benzene and 1,4-bis(2-(thiobenzoylthio)prop-2-yl)benzene as RAFT agents, respectively. Dually responsive multiblock copolymers were synthesized in a single aminolysis/oxidation step from the α,ω-bis(dithioester)-terminated PNIPAM and PDMAEMA. The copolymers and their stimulus-responsive behavior were characterized by size exclusion chromatography, NMR, light scattering and atomic force microscopy. Due to the presence of redox-sensitive disulfide bonds between the blocks, the copolymers were readily reduced to the starting polymer blocks. The presence of temperature-responsive PNIPAM blocks provided the copolymers with the ability to assemble into core-shell nanostructures with hydrophobic PNIPAM as a core and cationic PDMAEMA as stabilizing shell when above the phase transition temperatures of PNIPAM. The temperature-induced assembly of the copolymers also showed substantial pH sensitivity. The phase transition temperature increased with decreasing pH, while molecular weight of the assemblies decreased.

macromolecules

Dually Responsive Multiblock Copolymers via Reversible Addition−Fragmentation Chain Transfer Polymerization: Synthesis of Temperature- and Redox-Responsive Copolymers of Poly(<i>N</i>-isopropylacrylamide) and Poly(2-(dimethylamino)ethyl methacrylate)

Dually Responsive Multiblock Copolymers via Reversible Addition−Fragmentation Chain Transfer Polymerization: Synthesis of Temperature- and Redox-Responsive Copolymers of Poly(N-isopropylacrylamide) and Poly(2-(dimethylamino)ethyl methacrylate)