Strong Physical Hydrogels from Fibrillar Supramolecular Assemblies of Poly(ethylene glycol) Functionalized Hexaphenylbenzenes
2016
Marakis, J. | Wunderlich, K. | Klapper, M. | Vlassopoulos, D. | Fytas, G. | Müllen, K.
Gel formation without chemical cross-links requires strong physical bonds, as observed in diverse molecular and macromolecular systems or supramolecular assemblies above a critical concentration. Here, we present a new molecular amphiphile of propeller-like hexaphenylbenzene derivative bearing two short poly(ethylene glycol) (PEG) chains which forms reversible physical gels comprising long (∼2.2 μm) bundles of hydrogel fibrils in coexistence with spherical micelles. Combination of topological (entanglement-like) interactions between the fibers and specific hydrophobic interactions due to the helicity of the PEG chains is proposed to account for the hydrogelation in the semidilute regime. The present supramolecular hydrogels, which are based on small molecules, exhibit extraordinary properties with an exceptionally strong dependence of the shear modulus on concentration, akin to the behavior of ultrahigh molecular weight cellulose-based fibers.
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