Abstract
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.
Highlights
Several tissue-adhesive biomaterials have been proposed for surgical applications
We developed a novel hydrogel that covalently contains both a reactive polymeric micelle formed from poly-b-poly (PEG-PLA) block copolymers serving as a crosslinker and a polyamine as a main chain of the hydrogel [19]-[24] (Figure 1)
The hydrogel that was formed from the polymeric micelles possessing a highly packed inner core exhibited a higher storage modulus than the hydrogel that was formed from the polymeric micelles possessing a lowly packed structure
Summary
Several tissue-adhesive biomaterials have been proposed for surgical applications These materials have included fibrin glues [1] [2], collagen sheets with fibrin glues [3], fibrillar collagen [4], collagen with citric acid derivative [5], gelatin with resorcin and formalin [6], albumin with glutaraldehyde [7], cyanoacrylate [8], and synthetic polymers [9]-[12]. These materials have a number of disadvantages and need to be improved for clinical use. Complicated preparation procedures [9]-[12] required for some of the synthetic glues make their application difficult
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