Amphiphilic pH-responsive ABC triblock copolymers via RAFT-mediated aqueous PISA and comparison with their A-b-(B-co-C) diblock copolymer counterparts

[Display omitted] •Synthesis of pH-sensitive ABC triblock copolymers by RAFT-mediated aqueous PISA.•Comparison of PDMAm-b-PAA-b-PCMAm vs. PDMAm-b-P(CMAm-co-AA) copolymers.•A fully protonated intermediate PAA block favors higher order morphologies.•Spheres, worms and vesicles obtained for a single tr...

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Veröffentlicht in:European polymer journal 2024-03, Vol.208, p.112858, Article 112858
Hauptverfasser: Audureau, Nicolas, Coumes, Fanny, Guigner, Jean-Michel, Rieger, Jutta, Stoffelbach, François
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Sprache:eng
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Zusammenfassung:[Display omitted] •Synthesis of pH-sensitive ABC triblock copolymers by RAFT-mediated aqueous PISA.•Comparison of PDMAm-b-PAA-b-PCMAm vs. PDMAm-b-P(CMAm-co-AA) copolymers.•A fully protonated intermediate PAA block favors higher order morphologies.•Spheres, worms and vesicles obtained for a single triblock copolymer composition.•Crucial impact of spatial distribution of AA on morphology and pH responsiveness. The influence of the macroRAFT agent architecture on the morphology of the self-assemblies obtained by aqueous RAFT dispersion polymerization in PISA is studied by comparing amphiphilic AC, A(B-co-C) diblocks and ABC triblock copolymers, constituted of N,N-dimethylacrylamide (DMAm = A), acrylic acid (AA = B) and N-cyanomethylacrylamide (CMAm = C) monomer units. The aim of this study is to better understand the impact of the presence of pH-sensitive acrylic acid units and their spatial distribution in block copolymers. Generally, the presence of a fully protonated intermediate block of PAA between the two blocks (based on PDMAm and PCMAm) favors the formation of higher-order morphologies. These ABC triblock copolymers assemblies are pH-responsive and can undergo morphological transitions through the controlled deprotonation or protonation of the PAA segment, but do not completely dissociate at high pH (i.e. when AA units are fully ionized) unlike their A(B-co-C) diblock counterparts, where the pH-responsive monomer unit is homogeneously distributed within the solvophobic block.
ISSN:0014-3057
1873-1945
DOI:10.1016/j.eurpolymj.2024.112858