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Poly(N,N'-Diethylacrylamide)-Based Thermoresponsive Hydrogels with Double Network Structure.

Lenka Hanyková1, Ivan Krakovský1, Eliška Šestáková1

  • 1Department of Macromolecular Physics, Faculty of Mathematics and Physics, Charles University, V Holešovičkách 2, 180 00 Prague 8, Czech Republic.

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|October 30, 2020
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Summary

Double network (DN) hydrogels exhibit altered thermal sensitivity compared to single network (SN) hydrogels. DN hydrogels retain more bound water and show a broader, less intense phase transition, impacting drug release kinetics.

Keywords:
NMR spectroscopydifferential scanning calorimetrydouble networkpoly(N,N′-diethylacrylamide)swellingthermoresponsive hydrogel

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Area of Science:

  • Polymer Science
  • Materials Science
  • Physical Chemistry

Background:

  • Thermoresponsive hydrogels are crucial for controlled release applications.
  • Double network (DN) hydrogels offer tunable properties by combining different polymer networks.
  • Understanding the thermal response of DN hydrogels is key to optimizing their performance.

Purpose of the Study:

  • To investigate the temperature-dependent behavior of DN hydrogels composed of poly(N,N'-diethylacrylamide) (PDEAAm) and hydrophilic polymers (PAAm or PDMAAm).
  • To compare the thermal sensitivity and water interactions of DN hydrogels with single network (SN) hydrogels.
  • To develop a thermodynamic model for describing the deswelling behavior of these hydrogels.

Main Methods:

  • Swelling measurements
  • Differential scanning calorimetry (DSC)
  • 1H NMR and UV-Vis spectroscopies
  • Methylene blue release studies
  • Development of a van't Hoff analysis-based thermodynamic model

Main Results:

  • DN hydrogels displayed reduced deswelling intensity, smaller enthalpy and entropy changes, and a broader transition temperature range compared to SN hydrogels.
  • DN hydrogels retained significantly more bound water above the transition temperature due to interactions with the hydrophilic network.
  • NMR spectra revealed an abrupt transition, contrasting with swelling and DSC data.
  • Methylene blue release occurred on different timescales for SN and DN hydrogels.

Conclusions:

  • The hydrophilic network in DN hydrogels significantly modulates their thermal sensitivity and water binding capacity.
  • A new thermodynamic model was developed to quantify deswelling behavior and characterize water states in thermoresponsive hydrogels.
  • DN hydrogels present distinct advantages over SN hydrogels for applications requiring controlled water retention and release profiles.