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All-Polysaccharide, Self-Healing Injectable Hydrogels Based on Chitosan and Oxidized Hydroxypropyl Polysaccharides.

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This study presents a green method for creating polysaccharide hydrogels using dynamic imine bonds, avoiding toxic crosslinkers. These novel hydrogels offer tunable mechanical properties and rapid self-healing for various applications.

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Biomedical Engineering

Background:

  • Polysaccharide hydrogels are desirable for biomedical uses due to their biocompatibility and biodegradability.
  • Existing polysaccharide hydrogels often rely on small-molecule crosslinkers, which can cause toxicity or unwanted chemical modifications.
  • There is a need for safer, more efficient methods to produce functional polysaccharide hydrogels.

Purpose of the Study:

  • To develop a green, simple, and efficient strategy for preparing in situ forming polysaccharide hydrogels.
  • To create hydrogels using dynamic imine bonds formed between oxidized polysaccharides and chitosan, eliminating the need for small-molecule crosslinkers.
  • To investigate the properties and potential applications of these novel all-polysaccharide hydrogels.

Main Methods:

  • Chemoselective oxidation of oligo(hydroxypropyl)-substituted polysaccharides to introduce ketone groups.
  • Condensation of ketone groups with amine-containing moieties (chitosan) to form dynamic imine crosslinks.
  • Preparation of oxidized hydroxypropyl cellulose/chitosan (Ox-HPC-Chitosan) and oxidized hydroxypropyl dextran/chitosan (Ox-HPD-Chitosan) hydrogels.
  • Characterization of mechanical properties, swelling rates, and self-healing capabilities using rheometry.

Main Results:

  • Successfully prepared Ox-HPC-Chitosan and Ox-HPD-Chitosan hydrogels cross-linked via imine bonds.
  • Hydrogel storage modulus was tunable from 300 Pa to 13 kPa by controlling the degree of substitution of ketone groups.
  • Demonstrated rapid self-healing properties, high swelling rates, and facile injectability for the all-polysaccharide hydrogels.
  • The imine linkage provided pH responsiveness and potential for self-healing and injectability.

Conclusions:

  • A green and efficient strategy for constructing polysaccharide hydrogels without small-molecule crosslinkers was established.
  • The developed hydrogels exhibit tunable mechanical properties, rapid self-healing, and injectability, making them attractive for biomedical applications.
  • This approach offers a promising pathway for creating advanced hydrogels for biomedical, agricultural, and controlled release applications.