Glucosamine‐grafted methacrylated gelatin hydrogels as potential biomaterials for cartilage repair

Abstract

Glucosamine (GlcN) has been widely used to reduce joint pain and osteoarthritis progression, but the efficacy of GlcN remains controversial because of the low GlcN concentration reaching the articular cavity. The aim of this study is to provide an effective approach of GlcN delivery to a target site using photocrosslinkable methacrylated gelatin (GelMA)‐based hydrogels, where GlcN could be gradually released during the degradation of the GelMA hydrogel. Herein, GlcN was acrylated as the acryloyl glucosamine (AGA) and covalently grafted to GelMA, and more than 87.7% of 15% (w/v) GelMA hydrogel was grafted with AGA. Moreover, in vitro outgrowth and apoptosis assay of bone marrow stem cells (BMSCs) demonstrated that the GelMA–AGA hydrogels had better biocompatibility, larger cell attachment, and higher cell viability than pure GlcN and AGA materials. Also, 15% (w/v) GelMA–AGA hydrogel was injected into the defect site for in vivo rabbit cartilage repair. Compared with oral administration of pure GlcN and injection of pure GelMA, the repaired cartilages using GelMA–AGA hydrogels had the smoothest surface of the defect site, filling more than 95% defect bulk. The similar content of glycosaminoglycans to the native tissue and the maximum amount of type II collagen was found in the repaired cartilage using GelMA–AGA hydrogels, indicating the outgrowth of hyaline cartilage.

Advanced injectable hydrogels for cartilage tissue engineering

“…In addition, it is a key reagent for inducing chondrogenesis of MSCs in vitro ( García-Fernández et al, 2020 ; Wang et al, 2021e ; García-Couce et al, 2022 ). GlcN is a naturally occurring amino monosaccharide, widely used to reduce joint pain and repair cartilage ( Suo et al, 2020 ; Zhang et al, 2021c ). Quercetin and naringin are flavonoids widely found in fruits and vegetables with strong anti-inflammatory and antioxidant effects.…”

Polymeric Hydrogels for Controlled Drug Delivery to Treat Arthritis

“…Despite their advantages, gelatin-based hydrogels have certain shortcomings such as poor mechanical strength, low delivery efficacy, and difficulty in controlling drug release. To compensate for these shortcomings, modified gelatin hydrogels such as methacrylated gelatin (GelMA) [ 17 ]) and hybrid gelatin hydrogels prepared by cross-linking gelatin with natural polymers such as gelatin–hyaluronic acid [ 18 ], gelatin–chitosan [ 19 ], and gelatin–alginate [ 20 ] or with synthetic polymers such as gelatin–polyacrylamide [ 21 ] and gelatin–poly(vinyl alcohol) (PVA) [ 22 ] have been developed.…”

Hydrogels for Treatment of Different Degrees of Osteoarthritis

“…As another important component of glycosaminoglycan, glucosamine (GlcN) has been extensively used to reduce joint pain and slow the progression of osteoarthritis, while the stability of polysaccharide drugs remains a major problem in the treatment. Suo et al (2020a ) prepared photocrosslinkable methacrylated gelatin (GelMA)–based hydrogels by copolymerizing GlcN acrylic acid into acryloyl glucosamine and covalently grafting it into GelMA hydrogels.…”