Fracture of polymer-like networks with hybrid bond strengths

Abstract

The design and functionality of polymeric materials hinge on failure resistance. While molecular-level details drive crack evolution in polymer networks, the connection between individual chain scission and bulk failure remains unclear and difficult to probe. In this work, we systematically study the fracture mechanics of polymer-like networks with hybrid bond strengths. We reveal that varying the ratio of strong and weak strands within otherwise identical networks gives a non-monotonic relationship between intrinsic fracture energy and strong strand fraction. Networks with some weak strands can counterintuitively outperform those with exclusively strong strands. Experiments on poly(ethylene glycol) gels and architected polymer-like lattices together with simulations unveil these properties. We show through computational visualization that strand type concentrations impact crack growth patterns and fracture energy trends. Cracks propagate through weak layers at low strong strand fractions. Aggregate clusters deflect or pin cracks at similar concentrations of strong and weak strands. Cracks blunt due to dispersed weak strand failure at high strong strand fractions. The sacrificial weak strands can notably deconcentrate stress near the crack tip, which toughens by delaying crack advancement. The interplay between concentration and clustering of strand types in networks with hybrid bond strengths, combined with crack growth phenomena and nonlocal energy release, provides insights into unusual fracture characteristics. Results shed light on fracture in polymer networks and percolated lattices.