We have developed a hybrid hydrogel that is formed from a crosslinkable polymeric micelle and a
polyamine. Under optimal conditions, the hydrogel rapidly formed in one second after a crosslinkable
polymeric micelle solution was mixed with a polyamine solution. We could change the
hydrogel’s gelation properties, such as the storage modulus and gelation time by tuning the molecular
weights of block copolymers and by tuning the pH of the dissolving-solvent of the hydrogel’s
constituent components. Furthermore, we have clarified here that the structural difference among
the micelles acting as crosslinkers can affect the gelation properties of the hydrogel. According to
our findings, the hydrogel that was formed from the polymeric micelles possessing a highly
packed (i.e., well-entangled or crosslinked) inner core exhibited a higher storage modulus than
the hydrogel that was formed from the polymeric micelles possessing a lowly packed structure.
Our results demonstrate that a microscopic structural difference among crosslinkers can induce a
macroscopic change in the properties of the resulting hydrogels. For medical applications, the hydrogel
proposed in the present paper can encapsulate the hydrophobic compounds in crosslinkers
(polymeric micelles) so that the hydrogel can be available as the biomaterial for their sustained
release.
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