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Cited by 309

The DOI matches its Crossref record; 61 of the 61 references it cites were found in a registry or an index.

Thermo-responsive Diblock Copolymer Worm Gels in Non-polar Solvents

Open access
Fielding, Lee A., Lane, Jacob A., Derry, Matthew J., Mykhaylyk, Oleksandr O., Armes, Steven P.·2014·Journal of the American Chemical Society
DOI 10.1021/ja501756h
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Abstract

Benzyl methacrylate (BzMA) is polymerized using a poly(lauryl methacrylate) macromolecular chain transfer agent (PLMA macro-CTA) using reversible addition-fragmentation chain transfer (RAFT) polymerization at 70 °C in n-dodecane. This choice of solvent leads to an efficient dispersion polymerization, with polymerization-induced self-assembly (PISA) occurring via the growing PBzMA block to produce a range of PLMA-PBzMA diblock copolymer nano-objects, including spheres, worms, and vesicles. In the present study, particular attention is paid to the worm phase, which forms soft free-standing gels at 20 °C due to multiple inter-worm contacts. Such worm gels exhibit thermo-responsive behavior: heating above 50 °C causes degelation due to the onset of a worm-to-sphere transition. Degelation occurs because isotropic spheres interact with each other much less efficiently than the highly anisotropic worms. This worm-to-sphere thermal transition is essentially irreversible on heating a dilute solution (0.10% w/w) but is more or less reversible on heating a more concentrated dispersion (20% w/w). The relatively low volatility of n-dodecane facilitates variable-temperature rheological studies, which are consistent with eventual reconstitution of the worm phase on cooling to 20 °C. Variable-temperature (1)H NMR studies conducted in d26-dodecane confirm partial solvation of the PBzMA block at elevated temperature: surface plasticization of the worm cores is invoked to account for the observed change in morphology, because this is sufficient to increase the copolymer curvature and hence induce a worm-to-sphere transition. Small-angle X-ray scattering and TEM are used to investigate the structural changes that occur during the worm-to-sphere-to-worm thermal cycle; experiments conducted at 1.0 and 5.0% w/w demonstrate the concentration-dependent (ir)reversibility of these morphological transitions.

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Metadata

Authors
Fielding, L. A., Lane, J. A., Derry, M. J., Mykhaylyk, O. O., & Armes, S. P.
Venue
Journal of the American Chemical Society
Publisher
American Chemical Society (ACS)
Published
2014-04-08
Volume
136
Issue
15
Pages
5790-5798
ISSN
  • 0002-7863 (ISSN-L)
  • 1520-5126
DOI
10.1021/ja501756h
OpenAlex
W2091529380
Cited by
309
References
61
FWCI
15.03
Type
journal article
Language
en
Open access
hybrid

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