Influence of Epichlorohydrin Concentration on the Physicochemical and Rheological Performance of Lignin/PVA Hydrogels

This study investigates the influence of epichlorohydrin (EPCH) concentration on the rheological, mechanical, and swelling properties of lignin/PVA hydrogels. Hydrogels were prepared with EPCH concentrations ranging from 2.5% to 7.5%, and their viscoelastic properties were characterized through oscillatory strain and frequency sweep rheology. Increasing the EPCH concentration led to a substantial rise in mechanical stiffness, with the compressive modulus increasing from 21 kPa (2.5%) to 275 kPa (7.5%), accompanied by a marked reduction in swelling capacity from 460% to 190%. This behavior is attributed to the formation of a denser and more interconnected network structure with increasing cross-linking density. Furthermore, a strong correlation was observed between EPCH concentration and gelation kinetics, with higher concentrations generally leading to faster gelation times. In all formulations, gel time consistently decreased as the temperature increased from 10 to 50 °C. The optimal EPCH concentration for achieving a balance between mechanical properties and processability was determined to be 3.5%. At this concentration, the hydrogels exhibited a favorable combination of mechanical strength, shape recovery, and processability, while maintaining desirable swelling behavior. These findings provide valuable insights into the critical role of cross-linking density in determining the physicochemical properties of lignin/PVA hydrogels, paving the way for the development of these bio-based materials with tailored properties for diverse applications.