Abstract
AbstractIn recent years, new types of polymer gels have emerged, which have a well-controlled network structure and few topological defects. These so-called near-ideal polymer networks constitute a good model system to revisit the long-standing problem of structure–property relationships in polymer networks, as well as a promising platform for the development of polymer gels with outstanding mechanical properties. In this study, we investigate the relative contributions of network defects (dangling chains and second-order loops) on the stress–stretch response of near-ideal polymer networks using a computational discrete network model. We identify the average chain prestretch as a key parameter to capture the effect of network topology on the elastic modulus and maximum extensibility. Proper account of the chain prestretch further leads to scaling relations for the elastic properties in terms of topology parameters that differ from classical estimates of rubber elasticity theory. Stress–stretch curves calculated using the discrete network model are also compared to semi-analytical estimates.
Highlights
Soft polymeric materials such as elastomers and hydrogels are increasingly being developed for a broad range of applications in engineering and medicine
5 Conclusions We have developed a computational discrete network model to elucidate the effects of network parameters on the elasticity of near-ideal networks
Network parameters include the density of elastically-effective chains, average coordination of the junctions and loop fraction, which were all varied independently
Summary
Soft polymeric materials such as elastomers and hydrogels are increasingly being developed for a broad range of applications in engineering and medicine. The mechanical properties remains elusive [5] This is largely due to the fact that networks resulting from conventional random polymerisation and crosslinking processes have an irregular and spatially-heterogeneous structure, which is difficult to characterise and model [6, 7]. Near-ideal polymer networks have been introduced as a new concept for making soft materials with high stiffness and high strength [1,8,9]. The homogeneity of the network structure is believed to be the reason for the high stiffness and strength of tetra-arm hydrogels [8]. These hydrogels constitute promising model systems to revisit the fundamental question of topology-property relationships in polymer networks
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