Hybrid supramolecular and colloidal hydrogels that bridge multiple length scales.

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Janeček, Emma-Rose 
McKee, Jason R 
Tan, Cindy SY 
Nykänen, Antti 
Kettunen, Marjo 

Hybrid nanocomposites were constructed based on colloidal nanofibrillar hydrogels with interpenetrating supramolecular hydrogels, displaying enhanced rheological yield strain and a synergistic improvement in storage modulus. The supramolecular hydrogel consists of naphthyl-functionalized hydroxyethyl cellulose and a cationic polystyrene derivative decorated with methylviologen moieties, physically cross-linked with cucurbit[8]uril macrocyclic hosts. Fast exchange kinetics within the supramolecular system are enabled by reversible cross-linking through the binding of the naphthyl and viologen guests. The colloidal hydrogel consists of nanofibrillated cellulose that combines a mechanically strong nanofiber skeleton with a lateral fibrillar diameter of a few nanometers. The two networks interact through hydroxyethyl cellulose adsorption to the nanofibrillated cellulose surfaces. This work shows methods to bridge the length scales of molecular and colloidal hybrid hydrogels, resulting in synergy between reinforcement and dynamics.

hydrogels, nanocellulose, nanocomposites, supramolecular chemistry
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Angew Chem Int Ed Engl
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Engineering and Physical Sciences Research Council (EP/F035535/1)
European Research Council (240629)
This work was partially funded by the European Research CouncilStarting Investigator Grant (ASPiRe) ERC-2009-StG-240629, theEngineering and Physical Sciences Research Council grant EP/F035535/1, the ERC Advanced Grant ERC 2011-ADG 291364Mimefun, and the EPSRC. The Academy of Finland is acknowledgedthrough the Center of Excellence of Molecular Engineering ofBiosynthetic Hybrid Materials Research and an academy profes-sorship (O.I.). J.R.M. acknowledges the ESF Precision PolymerMaterials (P2M) network. O.I. and O.S. acknowledge the ESFPrecision Polymer Materials (P2M) network for initiation of thiswork. The Aalto Nanomicroscopy Center is acknowledged for use ofthe devices. C.S.Y.T. acknowledges funding from the Department ofHigher Education, Ministry of Education of Malaysia and theUniversiti Teknologi MARA (UiTM) of Malaysia.