Injectable spontaneously formed asymmetric adhesive hydrogel with controllable removal for wound healing

Healing large-scale wounds has been a long-standing challenge in the field of biomedicine. Herein, we propose an injectable oxidated sodium alginate/gelatin/3,3'-dithiobis(propionic hydrazide)-aurum (Alg-CHO/gelatin/DTPH-Au) hydrogel filler with asymmetric adhesion ability and removability, which is formed by the Schiff-base reaction between aldehyde-based sodium alginate and multi-amino crosslinkers (gelatin and DTPH), combined with the coordination interaction between Au nanoparticles and disulfide bond of DTPH. Consequently, the prepared Alg-CHO/gelatin/DTPH-Au hydrogel exhibits high mechanical properties and injectable behaviors owing to its multiple-crosslinked interactions. Moreover, because various types of interaction bonding form on the contact side with the tissue, denser crosslinking of the upper layer relative to the lower layer occurs. Combined with the temperature difference between the upper and lower surfaces, this results in asymmetric adhesive properties. Owing to the photothermal effect, the reversible coordination interaction between Au nanoparticles and DTPH and the change in the triple helix structure of gelatin to a coil structure impart the filler-phased removability and antibacterial ability. The choice of all natural polymers also allows for favorable degradability of the wound filler and outstanding biocompatibility. Based on these features, this versatile wound filler can achieve a wide range of applications in the field of all-skin wound repair.