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Reversible Addition-Fragmentation Chain Transfer Aqueous Dispersion Polymerization of 4-Hydroxybutyl Acrylate Produces Highly Thermoresponsive Diblock Copolymer Nano-Objects.
| Content Provider | Europe PMC |
|---|---|
| Author | Cumming, JulianaM. Deane, Oliver J. Armes, Steven P. |
| Copyright Year | 2022 |
| Abstract | Thereversible addition-fragmentation chain transfer (RAFT) aqueousdispersion polymerization of 2-hydroxypropyl methacrylate (HPMA) usinga poly(glycerol monomethacrylate) (PGMA) precursor is an importantprototypical example of polymerization-induced self-assembly. 4-Hydroxybutylacrylate (HBA) is a structural isomer of HPMA, but the former monomerexhibits appreciably higher aqueous solubility. For the two correspondinghomopolymers, PHBA is more weakly hydrophobic than PHPMA. Moreover,PHBA has a significantly lower glass transition temperature (Tg) so it exhibits much higher chain mobilitythan PHPMA at around ambient temperature. In view of these strikingdifferences, we have examined the RAFT aqueous dispersion polymerizationof HBA using a PGMA precursor with the aim of producing a series ofPGMA57–300-PHBA100–1580 diblockcopolymer nano-objects by systematic variation of the mean degreeof polymerization of each block. A pseudo-phase diagram is constructedusing transmission electron microscopy to assign the copolymer morphologyafter employing glutaraldehyde to cross-link the PHBA chains and henceprevent film formation during grid preparation. The thermoresponsivecharacter of the as-synthesized linear nano-objects is explored usingdynamic light scattering and temperature-dependent rheological measurements.Comparison with the analogous PGMAx-PHPMAy formulation is made where appropriate. Inparticular, we demonstrate that replacing the structure-directingPHPMA block with PHBA leads to significantly greater thermoresponsivebehavior over a much wider range of diblock copolymer compositions.Given that PGMA-PHPMA worm gels can induce stasis in human stem cells(see Canton et al., ACS Central Science, 2016, 2, 65–74), our findings are likelyto have implications for the design of next-generation PGMA-PHBA wormgels for cell biology applications. |
| Related Links | https://europepmc.org/backend/ptpmcrender.fcgi?accid=PMC9007527&blobtype=pdf |
| ISSN | 00249297 |
| Journal | Macromolecules |
| Volume Number | 55 |
| DOI | 10.1021/acs.macromol.1c02431 |
| PubMed Central reference number | PMC9007527 |
| Issue Number | 3 |
| PubMed reference number | 35431331 |
| e-ISSN | 15205835 |
| Language | English |
| Publisher | American Chemical Society |
| Publisher Date | 2022-01-19 |
| Access Restriction | Open |
| Rights License | Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). © 2022 American Chemical Society |
| Content Type | Text |
| Resource Type | Article |
| Subject | Organic Chemistry Materials Chemistry Inorganic Chemistry Polymers and Plastics |
