Efficient Catalyst-Free One-Pot Synthesis of Polysaccharide-Polypeptide Hydrogels in Aqueous Solution

Area of Science:

• Biomaterials Science
• Polymer Chemistry
• Nanotechnology

Background:

• Traditional polysaccharide-peptide hydrogel synthesis is complex and inefficient.
• Recent advances in aqueous ring-opening polymerization (ROP) and ROP-induced nanogelation offer new possibilities.

Purpose of the Study:

• To develop a simplified, one-pot aqueous strategy for synthesizing polysaccharide-polypeptide hydrogels.
• To explore the potential of these hydrogels in medical applications.

Main Methods:

• Aqueous ring-opening polymerization (ROP) of N-carboxyanhydride (NCA) initiated by carboxymethyl chitosan.
• Characterization of hydrogel properties, including elastic modulus, self-healing, injectability, swelling ratio, and biocompatibility.
• Investigation of the polymerization mechanism using morphology analysis.

Main Results:

• A catalyst-free, one-pot aqueous method successfully produced polysaccharide-polypeptide hydrogels.
• Hydrogel properties (elastic modulus 50–18000 Pa) were tunable by varying NCA type and amount.
• The hydrogels demonstrated self-healing, injectability, high swelling ratios (>95% water content), and excellent biocompatibility (low hemolysis and cytotoxicity).
• The polymerization followed a ring-opening polymerization-induced self-assembly (ROPISA) mechanism, with micelle aggregation driving gelation.

Conclusions:

• The developed aqueous one-pot strategy offers an effective and practical approach to synthesize tunable polysaccharide-polypeptide hydrogels.
• The hydrogels' self-healing, injectable, and biocompatible nature makes them highly promising for diverse medical applications.