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Polymers 2016, 8(3), 82;

Hybrid Polymer-Network Hydrogels with Tunable Mechanical Response

Institute of Chemistry and Biochemistry, Freie Universität Berlin, Takustr. 3, D-14195 Berlin, Germany
Soft Matter and Functional Materials, Helmholtz-Zentrum Berlin, Hahn-Meitner-Platz 1, D-14109 Berlin, Germany
These authors contributed equally to this work.
Author to whom correspondence should be addressed.
Academic Editor: André Laschewsky
Received: 6 February 2016 / Revised: 8 March 2016 / Accepted: 9 March 2016 / Published: 15 March 2016
(This article belongs to the Special Issue Polymers for Aqueous Media)
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Hybrid polymer-network gels built by both physical and covalent polymer crosslinking combine the advantages of both these crosslinking types: they exhibit high mechanical strength along with excellent fracture toughness and extensibility. If these materials are extensively deformed, their physical crosslinks can break such that strain energy is dissipated and irreversible fracturing is restricted to high strain only. This mechanism of energy dissipation is determined by the kinetics and thermodynamics of the physical crosslinking contribution. In this paper, we present a poly(ethylene glycol) (PEG) based material toolkit to control these contributions in a rational and custom fashion. We form well-defined covalent polymer-network gels with regularly distributed additional supramolecular mechanical fuse links, whose strength of connectivity can be tuned without affecting the primary polymer-network composition. This is possible because the supramolecular fuse links are based on terpyridine–metal complexation, such that the mere choice of the fuse-linking metal ion adjusts their kinetics and thermodynamics of complexation–decomplexation, which directly affects the mechanical properties of the hybrid gels. We use oscillatory shear rheology to demonstrate this rational control and enhancement of the mechanical properties of the hybrid gels. In addition, static light scattering reveals their highly regular and well-defined polymer-network structures. As a result of both, the present approach provides an easy and reliable concept for preparing hybrid polymer-network gels with rationally designed properties. View Full-Text
Keywords: hybrid polymer hydrogel; mechanical fuse links; model-network structure; poly(ethylene glycol) hybrid polymer hydrogel; mechanical fuse links; model-network structure; poly(ethylene glycol)

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Czarnecki, S.; Rossow, T.; Seiffert, S. Hybrid Polymer-Network Hydrogels with Tunable Mechanical Response. Polymers 2016, 8, 82.

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