Fracture Process of Double-Network Gels by Coarse-Grained Molecular Dynamics Simulation

Double-network (DN) gels consisting of highly and slightly cross-linked networks exhibit good mechanical properties, complicated deformation behavior, and fracture processes owing to the existence of a large number of influential parameters. To determine the effects of these factors at the molecular level to improve the mechanical properties further, we studied the fracture processes of DN gels using a coarse-grained molecular dynamics simulation. First, we propose a modeling method for DN gels consisting of highly (first) and slightly (second) cross-linked networks. Then, we stretch the DN gels and investigate the effects of the network ratio, chain length, and first- and second-network structures on the mechanical properties. During the stretching, the stress increases with the bond breaking in the first network. Then, the stress further increases with the simultaneous bond breaking in the first and second networks when they are entangled with one another. Finally, the bond breaking in the first network stops, and only the bond breaking in the second network occurs. The second network remains at a high strain, which prevents rupture of the gel. We find that (i) a low concentration of the first network is necessary for the gel to exhibit the properties of both the first and second networks, (ii) a tense first network increases the Young's modulus, and (iii) the second network with a long chain length and separated cross-linking points increases the peak stress and ductility. We have therefore successfully elucidated the effects of the network structures on the mechanical properties of DN gels.