Antibacterial Crosslinker for Ternary PCL-Reinforced Hydrogels Based on Chitosan, Polyvinyl Alcohol, and Gelatin for Tissue Engineering

Current hydrogels used for cartilage tissue engineering often lack the mechanical strength and structural integrity required to mimic native human cartilage. This study addresses this limitation by developing reinforced hydrogels based on a ternary polymer blend of poly(vinyl) alcohol (PVA), gelatin (GL), and chitosan (CH), with gentamicin sulfate (GS) as an antimicrobial agent and a crosslinker. The hydrogels were produced using two crosslinking methods, the freeze/thaw and heated cycles, and reinforced with forcespun polycaprolactone (PCL) nanofiber to improve mechanical performance. Chemical characterization revealed that GS forms weak hydrogen bonds with the ternary polymers, leading to esterification with PVA, and covalent bonds are formed as the result of the free amino group (-NH₂) of chitosan that reacts with the carboxylic acid group (-COOH) of gelatin. SEM images help us to see how the hydrogels are reinforced with polycaprolactone (PCL) fibers produced via force spinning technology, while mechanical properties were evaluated via uniaxial tensile and compressive tests. Water retention measurements were performed to examine the crosslinking process's influence on the hydrogel's water retention, while the hydrogel surface roughness was obtained via confocal microscopy images. A constitutive model based on non-Gaussian strain energy density was introduced to predict experimental mechanical behavior data of the hydrogel, considering a non-monotonous softening function. Loading and unloading tests demonstrated that GS enhanced crosslinking without compromising water retention or biocompatibility because of the reaction between the free amino group of CH and the carboxylic group of gelatin. The PCL-reinforced PVA/GL/CH hydrogel shows strong potential for cartilage repair and tissue engineering applications.