Electrospun fibrous membrane reinforced hydrogels with preferable mechanical and tribological performance as cartilage substitutes

Hydrogels have attracted much attention as cartilage substitutes due to their human tissue-like characteristics. However, developing cartilage substitutes require the combination of high mechanical strength and low friction. Despite great success in tough hydrogels, this combination was hardly realized. Inspired by the natural cartilage, electrospun fibrous membrane reinforced hydrogels with superior mechanical properties and low friction coefficient were designed using electrospinning, freeze-thawing, and annealing techniques. An ordered fibrous membrane was first constructed by electrospinning, in which the tensile strength and modulus have been improved successfully. Then the PVA/PAA/GO hydrogel was modified layer-by-layer by the multilayer ordered electrospun membrane of PVA/PAA/GO. The ordered fibrous membrane significantly enhanced the mechanical strength and friction properties in a manner that mimicked the collagen fibrils in the cartilage. When the number of the membranes was 4, the mechanical properties of the fibrous membrane reinforced hydrogel is maximized, which can be compared to natural cartilage, which can achieve a tensile strength of 13.7 ± 1.5 MPa, tensile modulus of 27.5 ± 3.2 MPa, compressive strength of 12.32 ± 1.35 MPa, compressive modulus of 20.35 ± 2.50 MPa. The ordered fibrous membrane endows the hydrogel with a higher tearing energy of 39.16 ± 4.05 KJ m^-2, which is the 5 times that of pure hydrogel (7.74 ± 0.86 KJ m^-2). In addition, the friction coefficient of the fibrous membrane reinforced hydrogel is as low as 0.039, 2 times smaller than that of the hydrogel without addition of the fibrous membrane. Therefore, such hydrogels had excellent mechanical properties and tribological properties, which could be widely used in tissue engineering such as in cartilage replacement.