Physically motivated models of polymer networks with dynamic cross-links: comparative study and future outlook

Abstract

Polymer networks consisting of a mixture of chemical and physical cross-links are known to exhibit complex time-dependent behaviour due to the kinetics of bond association and dissociation. In this article, we highlight and compare two recent physically based constitutive models that describe the nonlinear viscoelastic behaviour of such transient networks. These two models are developed independently by two groups of researchers using different mathematical formulations. Here, we show that this difference can be attributed to different viewpoints: Lagrangian versus Eulerian. We establish the equivalence of the two models under the special situation where chains obey Gaussian statistics and steady-state bond dynamics. We provide experimental data demonstrating that both models can accurately predict the time-dependent uniaxial behaviour of a poly(vinylalcohol) dual cross-link hydrogel. We review the advantages and disadvantages of both approaches in applications and close by discussing a list of open challenges and questions regarding the mathematical modelling of soft, viscoelastic networks.