One‐Pot Construction of Articular Cartilage‐Like Hydrogel Coating for Durable Aqueous Lubrication

Articular cartilage has an appropriate multilayer structure and superior tribological properties and provides a structural paradigm for design of lubricating materials. However, mimicking articular cartilage traits on prosthetic materials with durable lubrication remains a huge challenge. Herein, an ingenious three-in-one strategy is developed for constructing an articular cartilage-like bilayer hydrogel coating on the surface of ultra-high molecular weight polyethylene (BH-UPE), which makes full use of conceptions of interfacial interlinking, high-entanglement crosslinking, and interface-modulated polymerization. The hydrogel coating is tightly interlinked with UPE substrate through hydrogel-UPE interchain entanglement and bonding. The hydrogel chains are highly entangled with each other to form a dense tough layer with negligible hysteresis for load-bearing by reducing the amounts of crosslinker and hydrophilic initiator to p.p.m. levels. Meanwhile, the polymerization of monomers in the top surface region is suppressed via interface-modulated polymerization, thus introducing a porous surface for effective aqueous lubrication. As a result, BH-UPE exhibits an ultralow friction coefficient of 0.0048 during 10 000 cycles under a load of 0.9 MPa, demonstrating great potential as an advanced bearing material for disc prosthesis. This work may provide a new way to build stable bilayer coatings and have important implications for development of biological lubricating materials.