Abstract
Hydrogels comprise three-dimensional networks of hydrophilic polymers and have attracted considerable interest in various sectors, including the biomedical, pharmaceutical, agricultural, and food industries. These materials offer significant benefits for food packaging applications, such as high mechanical strength and excellent water absorption capacity, thereby contributing to the extension of product shelf life. Therefore, the aim of this study is to compare the performance of citric acid and glutaraldehyde as crosslinking agents in gelatine-based hydrogels reinforced with cellulose nanocrystals (CNC), contributing to the development of safe and environmentally responsible materials. The hydrogels were prepared using the casting method and characterised in terms of their physical, mechanical, and structural properties. The results indicated that hydrogels crosslinked with glutaraldehyde exhibited higher opacity, lower transparency, and greater mechanical strength, whereas those crosslinked with citric acid demonstrated improved clarity, reduced water permeability, and enhanced swelling capacity. The incorporation of CNC further improved mechanical strength, reduced weight loss, and altered both surface homogeneity and optical properties. Microstructural results obtained by SEM were consistent with the mechanical properties evaluated (TS, %E, and EM). The Gel-ca hydrogel displayed the highest elongation value (98%), reflecting better cohesion within the polymeric matrix. In contrast, films incorporating CNC exhibited greater roughness and cracking, which correlated with increased rigidity and mechanical strength, as evidenced by the high Young's modulus (420 MPa in Gel-ga-CNC2). These findings suggest that the heterogeneity and porosity induced by CNC limit the mobility of polymer chains, resulting in less flexible and more rigid structures. Additionally, the DSC analysis revealed that gelatine hydrogels did not exhibit a well-defined Tg, due to the predominance of crystalline domains. Systems crosslinked with citric acid showed greater thermal stability (higher Tm and ΔH(m) values), while those crosslinked with glutaraldehyde, although mechanically stronger, exhibited lower thermal stability. These results confirm the decisive effect of the crosslinking agent and CNC incorporation on the structural and thermal behaviour of hydrogels. In this context, the application of hydrogels in packaged products represents an eco-friendly alternative that enhances product presentation. This research supports the reduction in plastic consumption whilst promoting the principles of a circular economy and facilitating the development of materials with lower environmental impact.