Hydrogels composed of natural materials exhibit great application potential in artificial scaffolds for cartilage repair as they can resemble the extracellular matrices of cartilage tissues comprised of various glycosaminoglycan and collagen. Herein, the natural polymers with vinyl groups, i.e. maleilated chitosan (MCS) and methacrylated silk fibroin (MSF) micro/nanoparticles, were firstly synthesized. The chemical structures of MCS and MSF micro/nanoparticles were investigated using Fourier transform infrared (FTIR) spectroscopy, proton nuclear magnetic resonance (H NMR) spectroscopy, and X-ray photoelectron spectroscopy (XPS). Then MCS/MSF micro/nanocomposite hydrogels were prepared by the photocrosslinking of MCS and MSF micro/nanoparticles in aqueous solutions in the presence of the photoinitiator Darocur 2959 under UV light irradiation. A series of properties of the MCS/MSF micro/nanocomposite hydrogels including rheological property, equilibrium swelling, sol content, compressive modulus, and morphology were examined. The results showed that these behaviors could be tunable via the control of MSF content. When the MSF content was 0.1%, the hydrogel had the compressive modulus of 0.32±0.07MPa, which was in the range of that of articular cartilage. The in vitro cytotoxic evaluation and cell culture of the micro/nanocomposite hydrogels in combination with mouse articular chondrocytes were also investigated. The results demonstrated that the micro/nanocomposite hydrogels with TGF-β1 was biocompatible to mouse articular chondrocytes and could support cells attachment well, indicating their potential as tissue engineering scaffolds for cartilage repair.

Poly(vinyl alcohol) (PVA) hydrogels have been considered as promising implants for various soft tissue engineering applications because of their tissue-like viscoelasticity and biocompatibility. However, two critical barriers including lack of sufficient mechanical properties and non-tissue-adhesive characterization limit their application as tissue substitutes. Herein, PVA is methacrylated with ultralow degrees of substitution of methacryloyl groups to produce PVA-glycidyl methacrylate (GMA). Subsequently, the PVA-GMA/methacrylate-functionalized silica nanoparticle (MSi)-based nanocomposite hydrogels are developed via the photopolymerization approach. Interestingly, both PVA-GMA-based hydrogels and PVA-GMA/MSi-based nanocomposite hydrogels exhibit outstanding compressive properties, which cannot be damaged through compressive stress-strain tests in the allowable scope of a tensile tester. Moreover, PVA-GMA/MSi-based nanocomposite hydrogels demonstrate excellent tensile properties compared with neat PVA-GMA-based hydrogels, and 15-, 14-, and 24-fold increase in fracture stress, elastic modulus, and toughness, respectively, is achieved for the PVA-GMA/MSi-based hydrogels with 10 wt % of MSi. These remarkable enhancements can be ascribed to the amount of long and flexible polymer chains of PVA-GMA and the strong interactions between the MSi and PVA-GMA chains. More interestingly, exciting improvements in the cell adhesion can also be successfully achieved by the incorporation of MSi nanoparticles.

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Poly(vinyl alcohol) (PVA) hydrogels with high water content, good load‐bearing property, low frictional behavior as well as excellent biocompatibility have been considered as promising cartilage replacement materials. However, the lack of sufficient mechanical properties and cell adhesion are two critical barriers for their application as cartilage substitutes. To address these problems, herein, methacrylated PVA with low degree of substitution of methacryloyl group has been synthesized first. Then, methacrylated PVA‐glycidyl methacrylate/hydroxyapatite (PVA‐GMA/Hap) nanocomposite hydrogels have been developed by the photopolymerization approach subsequently. Markedly, both pure PVA‐GMA hydrogel and PVA‐GMA/Hap nanocomposite hydrogels exhibit excellent performance in compressive tests, and they are undamaged during compressive stress–strain tests. Moreover, compared to pure PVA‐GMA hydrogels, 8.5‐fold, 7.4‐fold, and 14.2‐fold increase in fracture stress, Young's modulus and toughness, respectively, can be obtained for PVA‐GMA/Hap nanocomposite hydrogels with 10 wt % Hap nanoparticles. These enhancements can be ascribed to the intrinsic property of PVA‐GMA and strong hydrogen bonding interactions between PVA‐GMA chain and Hap nanoparticles. More interestingly, significant improvement in the cell adhesion can also be successfully achieved by incorporation of Hap nanoparticles. These biocompatible nanocomposite hydrogels have great potential to be used as cartilage substitutes. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2019, 57, 1882–1889