Effect of Polymer Entanglement on the Toughening of Double Network Hydrogels

The mechanical strength of double network (DN) gels consisting of highly cross-linked poly(2-acrylamido-2-methylpropanesulfonic acid) (PAMPS) as the first component and linear polyacrylamide (PAAm) as the second component has been investigated by varying the molecular weight of the second polymer PAAm, Mw. The experimental results reveal that, for toughening of the DN gels, (1) Mw is one of the dominant parameters; (2) there is a critical value of Mw = 106 for a remarkable enhancement; (3) the fracture energy of DN gels with a Mw larger than 106 reaches a value as high as 103 J/m2. By plotting the strength of DN gels (fracture stress σ and fracture energy G) against a characteristic parameter of c[η], where c is the average concentration of PAAm in the DN gels and [η] is the intrinsic viscosity of PAAm, it is found that the dramatic increase in the mechanical strength of the DN gels occurs above the region where linear PAAm chains are entangled with each other. Thus, we conclude that the entanglement between the second component PAAm plays an important role of the toughening mechanism of DN gels. This result supports the heterogeneous model, which predicts the presence of "voids" of the first network PAMPS with a size much larger than the radius of the second polymer PAAm.