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Disulfide-Functionalized Diblock Copolymer Worm Gels.

Nicholas J Warren1, Julien Rosselgong1, Jeppe Madsen1

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Biomacromolecules
|July 14, 2015
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This summary is machine-generated.

Researchers developed disulfide-functionalized polymer worm gels using two RAFT polymerization strategies. Higher disulfide content created stronger gels, with one method yielding superior results and improved properties, demonstrating potential for enhanced biomaterials.

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Biomaterials Engineering

Background:

  • RAFT-synthesized diblock copolymer worms (poly(glycerol monomethacrylate)-poly(2-hydroxypropyl methacrylate), PGMA-PHPMA) are promising biomaterials.
  • Introducing disulfide groups can enhance gel properties through covalent crosslinking.
  • Controlling disulfide content and distribution is crucial for tailoring gel performance.

Purpose of the Study:

  • To investigate two distinct strategies for incorporating disulfide linkages into PGMA-PHPMA copolymer worms.
  • To evaluate the impact of varying disulfide content on the rheological properties and stability of the resulting worm gels.
  • To explore the potential of these disulfide-functionalized worm gels for biomimetic applications.

Main Methods:

  • Synthesis of disulfide-functionalized macro-CTAs using statistical copolymerization with disulfide dimethacrylate (DSDMA) or a disulfide-based bifunctional RAFT agent (DSDB).
  • RAFT aqueous dispersion polymerization of HPMA using binary mixtures of functionalized and non-functionalized macro-CTAs.
  • Oscillatory rheology to characterize gel strength and stability; reductive cleavage using TCEP to confirm disulfide bond reversibility.

Main Results:

  • Both strategies successfully produced disulfide-functionalized PGMA-PHPMA worm gels.
  • Increased disulfide content correlated with enhanced gel strength, attributed to inter-worm disulfide/thiol exchange crosslinking.
  • The DSDB-based macro-CTA yielded stronger gels and suppressed thermosensitivity but showed precipitation at higher concentrations compared to the DSDMA-based approach.

Conclusions:

  • Disulfide crosslinking via RAFT polymerization offers a tunable method for creating robust, biomimetic worm gels.
  • The choice of disulfide-functionalization strategy impacts gel properties, stability, and processing window.
  • Reductive cleavage of disulfide bonds demonstrates the reversible nature of the crosslinks, offering potential for dynamic biomaterial applications.