The preparation of polysaccharide-peptide hydrogels usually
involves
multiple synthetic steps, thus reducing the effectiveness and practicality
of these approaches. Inspired by recent discoveries in aqueous N-carboxyanhydride (NCA) ring-opening polymerization (ROP)
and ring-opening polymerization-induced nanogelation, we present an
aqueous one-pot strategy to prepare polysaccharide-polypeptide hydrogels.
In this study, water-soluble polysaccharide carboxymethyl chitosan
is used as the macromolecular initiator to prepare polysaccharide-polypeptide
copolymers through the aqueous ROP of NCA. The catalyst-free approach
afforded hydrogels with properties that could be controlled by adjusting
the type and amount of NCA used, with the elastic modulus ranging
from 50 Pa to 18000 Pa. The hydrogen bond-cross-linked hydrogel exhibited
self-healing and injectable properties. Morphology characterization
revealed that micelles were formed in the early stage of reaction,
suggesting that the polymerization follows an aqueous ring-opening
polymerization-induced self-assembly (ROPISA) mechanism and that aggregation
of micelles during the reaction caused the gelation. Moreover, the
hydrogels displayed high swelling ratios (>95% water content),
and
hemolysis and cytotoxicity experiments demonstrated that the hydrogels
had excellent biocompatibility, indicating their potential in medical
applications.