Hyperelastic constitutive modeling of hydrogels based on primary deformation modes and validation under 3D stress states

In isotropic linear elasticity, a constitutive model calibrated using a single deformation mode (e.g., compression or tension or shear) is sufficient to describe a complex three-dimensional (3D) stress state. Such an approach, however, is likely inadequate for modeling hydrogels, which exhibit a nonlinear stress-strain response that varies significantly between deformation modes and is also sensitive to microstructure via gel concentration. In this study, a combined experimental and constitutive modeling framework is proposed for the development and validation of concentration-dependent 3D hyperelastic models for hydrogels. Agarose hydrogel in a concentration range of 0.4–4% w/v is chosen as the model material. Uniaxial compression, uniaxial tension, and simple shear (three primary deformation modes) experiments are conducted. The small strain elastic modulus-gel concentration relationships obtained from experiments are compared with those predicted by the molecular theory of rigid polymer networks (Jones-Marques theory) to identify the concentration range in which entropic elastic (hyperelastic) response dominates. In this range (1.5–4% w/v), four hyperelastic constitutive models are fit to the combined compression-tension-shear stress-strain data: Mooney-Rivlin, three-parameter generalized Rivlin, Gent, and Gent-Gent models. It is demonstrated that the generalized Rivlin model offers the best overall accuracy, and the variation of its model parameters with gel concentration is consistent with the Jones-Marques theory. The resulting concentration-dependent Extended Generalized Rivlin model is employed in finite element simulations of the non-homogeneous 3D stress state of wedge indentation. Simulated load versus depth and strain field predictions show very good agreement with experimental wedge indentation results. Finally, it is shown that a hyperelastic model calibrated using only a single deformation mode yields poor results for other primary and 3D deformations, and thus multiple primary deformation modes (preferably all three) should be considered.