Cooperative dynamics of heuristic swelling and inhibitive micellization in double-network hydrogels by ionic dissociation of polyelectrolyte

In this study, a cooperative model has been proposed for the double network (DN) hydrogel, which synchronously undergoes heuristic swelling and inhibitive micellization by the ionic dissociation of polyelectrolyte. Flory-Huggins solution theory is initially employed to identify the working mechanism of dielectric constants on swelling behavior of the DN hydrogel. Then a free-energy function is introduced to formulate the constitutive relationship of the DN hydrogels, in which the first hydrotropic network undergoes a heuristic swelling and the second hydrophobic network undergoes an inhibitive micellization. Finally, the proposed model has been verified using the experimental results reported in the literature. A good agreement between the theoretical results and experimental ones has been achieved. This study provides a fundamental approach to formulate the constitutive relationship and to understand the cooperative dynamics of two types of networks in DN hydrogels induced by the polyelectrolyte.