The solvent effect modulates the formation of homogeneous polyphenol composite hydrogels with improved transparency...

The usage of delayed sternal closure films after thoracotomy surgery helps doctors deal with emergency conveniently. There is a growing demand to develop suturable, antibacterial and transparent films for delayed sternal closure. Although polyphenol incorporated hydrogels provide good suture ability, they lose transparency because of the heterogeneous distribution of polyphenols during the post-immersion process. Here, a solvent exchange method is proposed to fabricate homogeneous polyphenol composite hydrogels in a bottom-up manner, which utilizes the distinct solvent effect of DMSO and H₂O to modulate the association and disassociation between polyphenols and the polymer backbones on demand. DMSO first provides a protective environment to turn off the intermolecular interactions and allows tannic acid (TA) to be dispersed into the polymer network PEG-lysozyme (PEG-LZM) homogeneously. The following water rehydration turns on the intermolecular interactions between titanic acid and PEG-lysozymes, and results in a homogeneous titanic acid toughened composite hydrogel (PEG-LZM-TA (DH)), which has an improved transparency and mechanical properties than those of the materials prepared by the post-immersion method. In addition, the TA integration provides antibacterial function to the hydrogels. We establish a rabbit delayed sternal closure model to demonstrate that PEG-LZM-TA (DH) films can be sutured to temporarily close the thoracic cavity of rabbits, provide a transparent window to inspect the wound at any time, and control the bacterial contamination efficiently. We further explore the solvent exchange method to other polyphenols and polymeric hydrogel composites. The results suggest that the solvent exchange method provides generic opportunities to fabricate homogeneous polyphenol strengthened hydrogel systems with high performance.