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Highly Entangled Hydrogels by Photoiniferter-Mediated Polymerization.

Gavin Irvine1, Konstantinos Myronidis2, Fulvio Pinto2

  • 1Department of Chemistry, University of Bath, Claverton Down, Bath, BA2 7AY, UK.

Angewandte Chemie (International Ed. in English)
|February 12, 2025
PubMed
Summary
This summary is machine-generated.

We synthesized ultra-high molecular weight poly(N,N-dimethylacrylamide) hydrogels using reversible deactivation radical polymerization. These highly entangled polymer networks exhibit enhanced toughness and swelling resistance, even with minimal crosslinking.

Keywords:
RAFTentanglementshydrogelspolymer networksrheology

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Area of Science:

  • Polymer Chemistry
  • Materials Science
  • Supramolecular Chemistry

Background:

  • Hydrogels are crucial in various applications, but achieving high toughness and swelling resistance often requires high crosslinking densities.
  • Controlling polymer chain architecture and entanglement is key to designing advanced hydrogel properties.
  • Reversible deactivation radical polymerization (RDRP) offers precise control over polymer chain growth and architecture.

Purpose of the Study:

  • To synthesize ultra-high molecular weight (UHMW) poly(N,N-dimethylacrylamide) (PDMAm) hydrogels with extremely low crosslinking densities.
  • To investigate the simultaneous control over crosslinking density and primary chain molecular weight.
  • To explore the role of polymer chain entanglements in dictating hydrogel properties.

Main Methods:

  • Utilized trithiocarbonate photoiniferter-mediated RDRP for controlled synthesis of PDMAm chains.
  • Systematically varied the targeted degree of polymerization (DPtarget) while maintaining a fixed photoiniferter to crosslinker ratio.
  • Characterized hydrogel properties, including storage modulus (G') and swelling behavior, in relation to polymer architecture.

Main Results:

  • Achieved UHMW PDMAm hydrogels with vanishingly small crosslinking densities.
  • Observed a transition to an entanglement-dominated regime for DPtarget > 5,000, indicated by a plateau in storage moduli.
  • Demonstrated enhanced toughness and swelling resistance in highly entangled hydrogels, outperforming those reliant on covalent crosslinks.

Conclusions:

  • Developed a facile method for synthesizing elastic and tough hydrogels with tunable contributions from entanglements and crosslinks.
  • Showcased the potential of dense polymer chain entanglements to act as effective transient crosslinks, enhancing hydrogel stability.
  • Established a structure-property relationship where high molecular weight chains and entanglements significantly improve hydrogel performance.