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Valeriya S Kukanova1, Hanna A Zhurauleva2, Sergei V Kostjuk3

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This study introduces a novel thermoresponsive graft copolymer, P(NIPAM-g-PLA), for injectable hydrogels. Its unique gelation mechanism, separate from coil-to-globule transitions, and aging effects are crucial for biomedical applications.

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Area of Science:

  • Polymer Science
  • Biomaterials Engineering
  • Materials Chemistry

Background:

  • Thermoresponsive polymers are key for injectable hydrogels, typically relying on coil-to-globule transitions for gelation.
  • Distinct gelation mechanisms beyond coil-to-globule transitions are often overlooked in hydrogel design.
  • Understanding these mechanisms is vital for optimizing hydrogel properties for biomedical use.

Purpose of the Study:

  • To investigate a novel graft copolymer, P(NIPAM-g-PLA), with a distinct thermoresponsive gelation mechanism.
  • To characterize the phase behavior and gelation properties of P(NIPAM-g-PLA) in aqueous solutions.
  • To evaluate the impact of polymer concentration, temperature, and buffer solutions on gelation and injectability.

Main Methods:

  • Synthesis and characterization of P(NIPAM-g-PLA) graft copolymer.
  • Rheological measurements to determine gelation temperatures (Tgel) and binodal temperatures (Tb).
  • Phase behavior analysis across different temperatures and concentrations, including in phosphate-buffered saline (PBS).

Main Results:

  • P(NIPAM-g-PLA) exhibits a unique gelation mechanism where Tgel is distinct from Tb, allowing for transparent gel formation.
  • The system displays four phases: transparent sol, opaque sol, transparent gel, and opaque gel.
  • Gelation is concentration-dependent, with injectability limited around 10 wt%; aging leads to complete loss of gelation ability.

Conclusions:

  • P(NIPAM-g-PLA) offers a novel approach to thermoresponsive hydrogel design with separate gelation and phase separation processes.
  • The distinct gelation mechanism, potentially involving physical cross-linking of hydrophobic 'pearls', provides tunable hydrogel properties.
  • Consideration of buffer effects and long-term polymer aging is essential for developing reliable injectable hydrogels for biomedical applications.