Synergistic Anti-inflammatory Coating "Zipped Up" on Polypropylene Hernia Mesh

Violent inflammation has impeded worry-free application of polypropylene (PP) hernia meshes. Efficient anti-inflammatory coatings are urgently needed to alter the situation. Here, we present a zipper-like, two-layer coating with an intermediate antioxidant layer (I) and an outer antifouling layer (II) to endow PP meshes with synergistic anti-inflammatory effects. The controllable antioxidant ability of layer I was obtained by modulating the assembly cycle of the metal-phenolic network (MPN) composed of tannic acid (TA) and Fe³⁺. Polyzwitterionic (PMAD) brush-based layer II was generated upon multiple interactions between the catechol side groups of PMAD and layer I. To consolidate the entire assembly architecture, aryloxy radical coupling was initiated through alkali-catalyzed oxidation. The reaction is similar to a "zipping up" process to construct covalent bonds in the I-II interface and layer I by coupling adjacent catechol groups, which facilely achieved grafting and cross-linking. The obtained coating (PMAD-TA/Fe) did not affect the original properties of the PP mesh and remained stable during cyclic tensile testing or degradation. Most importantly, the excellent antioxidant and antifouling capacities enabled PMAD-TA/Fe-PP to exhibit desirable anti-inflammatory effects and reduce collagen deposition when compared with the bare material. The synergistic anti-inflammatory coating eliminates a major hindrance in the design of biocompatible meshes, and its potential application in developing medical implants with low immunogenicity is promising.