Tough, Slippery, and Low-Permeability Multilayer Hydrogels Modified by Anisotropic Fiber Membrane for Soft Tissue Replacement
Xinyue Zhang, Qin Chen, Kai Chen, Haiyan Feng, Cunao Feng, Xiaowei Li, Dekun Zhang, Shirong Ge
Abstract
Hydrogels with sustained lubrication, high load-bearing capacity, and wear resistance are essential for applications in soft tissue replacements and soft material devices. Traditional tough or lubricious hydrogels fail to balance the lubrication and load-bearing functions. Inspired by the gradient-ordered multilayer structures of natural tissues (such as cartilage and ligaments), a tough, smooth, low-permeability, and low-friction anisotropic layered electrospun fiber membrane-reinforced hydrogel was developed using electrospinning and annealing recrystallization. This hydrogel features a stratified porous network structure of varying sizes with tightly bonded interfaces, achieving an interfacial bonding toughness of 1.6 × 10 3 J/m 2 . The anisotropic fiber membranes, mimicking the orderly fiber structures within soft tissues, significantly enhance the mechanical properties of the hydrogel with a fracture strength of 20.95 MPa, a Young’s modulus of 29.64 MPa, and a tear toughness of 37.94 kJ/m 2 and reduce its permeability coefficient (6.1 × 10 –17 m 4 N –1 s –1 ). Meanwhile, the hydrogel demonstrates excellent solid–liquid phase load-bearing characteristics, which can markedly improve the tribological performance. Under a contact load of 4.1 MPa, the anisotropic fiber membrane-reinforced hydrogel achieves a friction coefficient of 0.036, a 219% reduction compared with pure hydrogels. Thus, the superior load-bearing and lubricating properties of this layered hydrogel underscore its potential applications in soft tissue replacements, medical implants, and other biomedical devices.