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ACS Nano. 2016 Jan 26;10(1):1317-24. doi: 10.1021/acsnano.5b06692. Epub 2016 Jan 7.

Controlling Hydrogel Mechanics via Bio-Inspired Polymer-Nanoparticle Bond Dynamics.

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Department of Materials Science and Engineering, Massachusetts Institute of Technology , 77 Massachusetts Avenue, Cambridge, Massachusetts 02139, United States.
Chemistry of Life Processes Institute, Northwestern University , Evanston, Illinois 60208, United States.
Department of Bioengineering and Materials Science and Engineering, University of California, Berkeley , 210 Hearst Mining Building, Berkeley, California 94720-1760, United States.


Interactions between polymer molecules and inorganic nanoparticles can play a dominant role in nanocomposite material mechanics, yet control of such interfacial interaction dynamics remains a significant challenge particularly in water. This study presents insights on how to engineer hydrogel material mechanics via nanoparticle interface-controlled cross-link dynamics. Inspired by the adhesive chemistry in mussel threads, we have incorporated iron oxide nanoparticles (Fe3O4 NPs) into a catechol-modified polymer network to obtain hydrogels cross-linked via reversible metal-coordination bonds at Fe3O4 NP surfaces. Unique material mechanics result from the supra-molecular cross-link structure dynamics in the gels; in contrast to the previously reported fluid-like dynamics of transient catechol-Fe(3+) cross-links, the catechol-Fe3O4 NP structures provide solid-like yet reversible hydrogel mechanics. The structurally controlled hierarchical mechanics presented here suggest how to develop hydrogels with remote-controlled self-healing dynamics.


bio-inspired metal-coordinate polymers; nanocomposite hydrogels; organic−inorganic interface; polymer physics; rheology; supra-molecular assembly

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