A unified viscoelastic constitutive model for studying the mechanical behaviors of polyelectrolyte complex hydrogels with different crosslinker degrees

Bio-based hydrogels formed by the chemically or physically cross-links are promising materials in the biological system. In this paper, we propose a constitutive model within the framework of finite-strain viscoelasticity to investigate the mechanical behaviors of bio-based polyelectrolyte complex (PEC) hydrogels from the ionic complexation of sodium hyaluronate (HA)/chitosan with and without chemical crosslinkers. The structure of the viscoelastic constitutive model consists of a spring and a Kelvin element, in which two softening factors are adopted to represent the states of ionic bonds and bridges in the hydrogels. Based on some constitutive assumptions and through the conventional approach of thermodynamics, the constitutive equation system of the model is derived. Corresponding to the hydrogels with different crosslinker concentrations, the values of material parameters in the model are identified. To show the validity of the model, it is applied to simulate the mechanical behaviors of the hydrogel samples in the uniaxial tensile tests and cyclic loading-unloading tests. It is found that the model predictions can fit the experimental data quite well. Based on the modeling results, some further analyses regarding the effects of softening factors on the response of HA/chitosan hydrogels have also been conducted.