Zwitterionic Poly‐Carboxybetaine Polymers Restore Lubrication of Inflamed Articular Cartilage

Abstract Osteoarthritis is a degenerative joint disease that is associated with decreased synovial fluid viscosity and increased cartilage friction. Though viscosupplements are available for decades, their clinical efficacy is limited and there is ample need for more effective joint lubricants. This study first evaluates the tribological and biochemical properties of bovine articular cartilage explants after stimulation with the inflammatory cytokine interleukin‐1β. This model is then used to investigate the tribological potential of carboxybetaine (CBAA)‐based zwitterionic polymers of linear and bottlebrush architecture. Due to their affinity for cartilage tissue, these polymers form a highly hydrated surface layer that decreases friction under high load in the boundary lubrication regime. For linear pCBAA, these benefits are retained over several weeks and the relaxation time of cartilage explants under compression is furthermore decreased, thereby potentially boosting the weeping lubrication mechanism. Bottlebrush bb‐pCBAA shows smaller benefits under boundary lubrication but is more viscous than linear pCBAA, therefore providing better lubrication under low load in the fluid‐film regime and enabling a longer residence time to bind to the cartilage surface. Showing how CBAA‐based polymers restore the lost lubrication mechanisms during inflammation can inspire the next steps toward more effective joint lubricants in the future.