A theory of finite tensile deformation of double‐network hydrogels

Abstract A continuum damage model was developed to describe the finite tensile deformation of tough double‐network (DN) hydrogels synthesized by polymerization of a water‐soluble monomer inside a highly crosslinked rigid polyelectrolyte network. Damage evolution in DN hydrogels was characterized by performing loading‐unloading tensile tests and oscillatory shear rheometry on DN hydrogels synthesized from 3‐sulfopropyl acrylate potassium salt (SAPS) and acrylamide (AAm). The model can explain all the mechanical features of finite tensile deformation of DN hydrogels, including idealized Mullins effect and permanent set observed after unloading, qualitatively and quantitatively. The constitutive equation can describe the finite elasto‐plastic tensile behavior of DN hydrogels without resorting to a yield function. It was showed that tensile mechanics of DN hydrogels in the model is controlled by two material parameters which are related to the elastic moduli of first and second networks. In effect, the ratio of these two parameters is a dimensionless number that controls the behavior of material. The model can capture the stable branch of material response during neck propagation where engineering stress becomes constant. Consistent with experimental data, by increasing the elastic modulus of the second network the finite tensile behavior of the DN hydrogel changes from necking to strain hardening.