Mechanically Robust Lubricating Hydrogels Contrived by Harnessing Low‐Entropy Nanocrystalline Polymer Network

作者：Danli Hu, Yuke Yan, Wan‐Xin Wei, Changcheng Bai, Yaozhong Lu, Yixian Wang, Fei Zhai, Desheng Liu, Xiaolong Wang · 发表于：Advanced Functional Materials · 年份：2025 · DOI：10.1002/adfm.202508450 · 被引用次数：26 · 研究领域：Advancements in Transdermal Drug Delivery、Hydrogels: synthesis, properties, applications、Lubricants and Their Additives

Abstract Hydrogels with extraordinary mechanics hold tremendous application prospects in the field of artificial human load‐bearing tissues, but the invention of cartilage‐like hydrogels with unprecedented mechanical robustness and dependable lubricity is still a substantial challenge. Herein, a low‐entropy nanocrystalline domains network control strategy is proposed to construct mechanically robust poly (vinyl alcohol)/chitosan (PVA/CS) hydrogels with superior and durable lubrication performance. Consequently, the resulting PVA/CS hydrogels feature tunable mechanical performance by altering interaction between PVA and CS in the polymer network, spanning fracture strength, elastic modulus, toughness, and stretchability. Furthermore, its friction coefficient against the Al 2 O 3 ball keeps as low as 0.034 for 1 × 10 5 reciprocating cycles at 5 N, 1 Hz with water as the tribological medium, and even no destructive wear is found after friction test. To exploit the applications, PVA/CS hydrogels are processed into a femoral head and rubbed against swine acetabulum and found to have comparable lubricating properties to natural animal cartilage, positioning it as a superior competitor within the realm of durable lubricating hydrogel systems. This work corroborates the supposition that inducing polymer chains to form low‐entropy nanocrystalline domain structures is able to yield robust hydrogels with extraordinarily enhanced mechanical performances.