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Keywords:

  • Click chemistry;
  • Gels;
  • Magnetic materials;
  • Nanoparticles, magnetic;
  • Polymer composites;
  • Polymer gels;
  • Supramolecular materials

Abstract

Supramolecular gels consisting of trivalent polyisobutylene and bivalent poly(ethylene oxide) are generated. Strong hydrogen bonding interactions, affixed to the end-group moieties of the respective polymers (binding constant Kassn = 105M–1), serve as molecular glue, leading to the formation of weak gels. Two different gels were prepared: one, with a short telechelic poly(ethylene glycol) (PEG) segment (gel A), and one with a longer PEG segment (number-average molecular weight Mn = 2000 g mol–1) (gel B). Both gels show a significant increase in viscosity upon mixing of the two polymeric components, with a lag time of several minutes, indicative of nucleation mechanisms as the formation principle. However, only gel A displays classical gel-like behavior, with a loss modulus G′ larger than the storage modulus G″ after formation. Both gels display microphase-separated behavior with a spacing between 4–5 nm as probed via small-angle X-ray scattering (SAXS) and transmission electron microscopy (TEM) measurements. The incorporation of magnetic nanoparticles (Fe2O3; radius r = 3.5 nm) is successfully achieved, generating new magnetic gels with strongly thermoresponsive properties, displaying a strong temperature-dependent release profile of included dye molecules. Magnetic measurements indicate a superparamagnetic behavior of the incorporated nanoparticles, prospecting the application as magneto-sensitive delivery gels for pharmaceutical purposes.