Self‐Healing Gelatin Hydrogels Cross‐Linked by Combining Multiple Hydrogen Bonding and Ionic Coordination

Self‐healing hydrogels have been studied by many researchers via multiple cross‐linking approaches including physical and chemical interactions. It is an interesting project in multifunctional hydrogel exploration that a water soluble polymer matrix is cross‐linked by combining the ionic coordination and the multiple hydrogen bonds to fabricate self‐healing hydrogels with injectable property. This study introduces a general procedure of preparing the hydrogels (termed gelatin‐UPy‐Fe) cross‐linked by both ionic coordination of Fe3+ and carboxyl group from the gelatin and the quadruple hydrogen bonding interaction from the ureido‐pyrimidinone (UPy) dimers. The gelatin‐UPy‐Fe hydrogels possess an excellent self‐healing property. The effects of the ionic coordination of Fe3+ and quadruple hydrogen bonding of UPy on the formation and mechanical behavior of the prepared hydrogels are investigated. In vitro drug release of the gelatin‐UPy‐Fe hydrogels is also observed, giving an intriguing glimpse into possible biological applications. Dual physically cross‐linked hydrogels with excellent self‐healing property and injection possibility are prepared by virtue of multiple hydrogen bonding and ionic interactions. The ionic interaction contributes to the strength of the prepared hydrogel, while the multiple hydrogen bonding facilitates its self‐healing ability after damage. This work provides an innovative strategy to fabricate injectable hydrogels with self‐healing property.