Unlocking the potential of polymer networks for high strength through topology

Abstract

A covalent polymer network is orders of magnitude weaker than individual covalent bonds. This large gap reveals an unrealized potential. The weakness of a network comes not from individual covalent bonds, but from how they are connected. Here we unlock this potential by identifying a topological criterion, involving optimally sparse crosslinks, long chains, and dense entanglements. Optimizing each topological variable alone is insufficient for high strength, yet exceptional strength emerges when they are combined within a narrow regime. We describe the physics of this synergy, and use the criterion to strengthen networks widely used but known to be weak. For example, we prepare a polyacrylamide hydrogel of 90 wt% water, amplifying strength from a commonly reported value of ~0.1 MPa to ~6.5 MPa. The exceptional strength is achieved without sacrificing other properties, such as softness, toughness, and elasticity. The criterion establishes topology as a general design principle for strong polymer networks.