Cartilage-Inspired Hydrogel with Mechanical Adaptability, Controllable Lubrication, and Inflammation Regulation Abilities

Cartilage is a key component in joints because of its load-bearing and lubricating abilities. However, osteoarthritis often leads to afunction of load-bearing/lubrication and occurrence of inflammation with overexpressed reactive oxygen species (ROS) and nitric oxide (NO). To address these issues, we fabricated a novel polyanionic hydrogel with abundant carboxylates/sulfonates ("CS" hydrogel), inspired by normal cartilage rich in anionic hyaluronate/sulfonate glycosaminoglycan/lubricin, and crosslinked it tightly by Fe³⁺ ("CS-Fe" hydrogel). The "CS-Fe" hydrogel displayed mechanical adaptability and shear resistance. A low coefficient of friction (∼0.02) appeared when a loose hydrogel layer was generated because of the photoreduction of Fe³⁺ to Fe²⁺ by UV irradiation. This biocompatible "CS-Fe" hydrogel suppressed the overexpressed hydroxyl radical (·OH) and NO in macrophages and protected chondrocytes/fibroblasts from aggressive inflammation. Moreover, the layered "CS-Fe" hydrogel avoided cell death of chondrocytes in sliding tests. The results demonstrate that this cartilage-inspired hydrogel is a promising candidate material in cartilage tissue engineering to especially address inflammation.