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Simultaneous Formation of Polyhydroxyurethanes and Multicomponent Semi-IPN Hydrogels.

Ana I Carbajo-Gordillo1, Elena Benito1, Elsa Galbis1

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Summary

This study presents a novel, single-step method for creating advanced polyhydroxyurethane (PHU) hydrogels using Non-Isocyanate Polyurethane (NIPU) chemistry. The resulting PHU-PVA/gelatin hydrogels show enhanced rheological and mechanical properties for biomedical applications.

Keywords:
IPNNIPUPHUSIPNcyclic carbonatesfunctional polymersinterpenetrated networksporous materialsrheological properties

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Biomedical Engineering

Background:

  • Development of advanced hydrogel materials with tunable properties is crucial for biomedical applications.
  • Existing synthesis methods for polyhydroxyurethane (PHU) hydrogels can be complex and lack orthogonality.
  • Non-Isocyanate Polyurethane (NIPU) chemistry offers a safer and potentially more versatile alternative for polymer synthesis.

Purpose of the Study:

  • To develop an efficient, single-step strategy for synthesizing multicomponent polyhydroxyurethane-based hydrogels.
  • To investigate the impact of Non-Isocyanate Polyurethane (NIPU) synthesis on hydrogel properties.
  • To explore the potential of these hydrogels in biomedical applications.

Main Methods:

  • Synthesized crosslinked polyhydroxyurethane (PHU) using Non-Isocyanate Polyurethane (NIPU) methodology via aminolysis of bis(cyclic carbonate) (bisCC) monomers.
  • Formed Semi-Interpenetrating Network (SIPN) hydrogels by growing PHU within Polymer 2 (PVA or gelatin) colloidal solutions.
  • Optimized PHU formation through a 20-trial methodology, evaluating polymer concentration, temperature, solvent, and catalyst (thiourea derivative [TU] and 1,8-diazabicyclo [5.4.0]undec-7-ene [DBU]).

Main Results:

  • Achieved high molecular weights for PHU under optimized conditions, with monomer E-based PHU showing higher molecular weight (34.1 kDa) than monomer A-based PHU (16.4 kDa).
  • PVA-based hydrogels exhibited superior solid-like gel behavior and enhanced mechanical properties and elasticity, particularly when using monomer E.
  • SEM analysis revealed distinct microstructures, including superporous sponge-like patterns in certain PVA/monomer A hydrogels.

Conclusions:

  • The developed NIPU-based strategy provides an efficient, single-step method for creating advanced multicomponent hydrogels.
  • The synthesized hydrogels demonstrate tunable rheological and mechanical properties, with PVA-based systems showing promising performance.
  • This versatile methodology holds significant potential for diverse biomedical applications.