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Reversible crosslinking is a design paradigm for polymeric materials, whereinthey are microscopically reinforced with chemical species that form transientcrosslinks between the polymer chains. Besides the potential for self-healing,recent experimental work suggests that freely diffusing reversible crosslinksin polymer networks, such as gels, can enhance the toughness of the materialwithout substantial change in elasticity. This presents the opportunity formaking highly elastic materials that can be strained to a large extent beforerupturing. Here, we employ Gaussian chain theory, molecular simulation, andpolymer self-consistent field theory for networks to construct an equilibriumpicture for how reversible crosslinks can toughen a polymer network withoutaffecting its linear elasticity. Maximisation of polymer entropy drives thereversible crosslinks to bind preferentially near the permanent crosslinks inthe network, leading to local molecular reinforcement without significantalteration of the network topology. In equilibrium conditions, permanentcrosslinks share effectively the load with neighbouring reversible crosslinks,forming multi-functional crosslink points. The network is thereby globallytoughened, while the linear elasticity is left largely unaltered. Practicalguidelines are proposed to optimise this design in experiment, along with adiscussion of key kinetic and timescale considerations.

Harnessing entropy to enhance toughness in reversibly crosslinked polymer networks