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Issue 11, 2014
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Simple approach to reinforce hydrogels with cellulose nanocrystals

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The physical crosslinking of colloidal nanoparticles via dynamic and directional non-covalent interactions has led to significant advances in composite hydrogels. In this paper, we report a simple approach to fabricate tough, stretchable and hysteretic isotropic nanocomposite hydrogels, where rod-like cellulose nanocrystals (CNCs) are encapsulated by flexible polymer chains of poly(N,N-dimethylacrylamide) (PDMA). The CNC–PDMA colloidal clusters build a homogeneously cross-linked network and lead to significant reinforcing effect of the composites. Hierarchically structured CNC–PDMA clusters, from isolated particles to an interpenetrated network, are observed by transmission electron microscopy measurements. Dynamic shear oscillation measurements are applied to demystify the differences in network rheological behaviors, which were compared with network behaviors of chemically cross-linked PDMA counterparts. Tensile tests indicate that the hybrid hydrogels possess higher mechanical properties and a more efficient energy dissipation mechanism. In particular, with only 0.8 wt% of CNC loading, a 4.8-fold increase in Young's modulus, 9.2-fold increase in tensile strength, and 5.8-fold increase in fracture strain are achieved, which is ascribed to a combination of CNC reinforcement in the soft matrix and CNC–PDMA colloidal cluster conformational rearrangement under stretching. Physical interactions within networks serve as reversible sacrificial bonds that dissociate upon deformation, exhibiting large hysteresis as an energy dissipation mechanism via cluster mobility. This result contrasts with the case of chemically cross-linked PDMA counterparts where the stress relaxation is slow due to the permanent cross-links and low resistance against crack propagation within the covalent network.

Graphical abstract: Simple approach to reinforce hydrogels with cellulose nanocrystals

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Publication details

The article was received on 05 Mar 2014, accepted on 28 Mar 2014 and first published on 01 Apr 2014

Article type: Paper
DOI: 10.1039/C4NR01214C
Nanoscale, 2014,6, 5934-5943

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    Simple approach to reinforce hydrogels with cellulose nanocrystals

    J. Yang, C. Han, F. Xu and R. Sun, Nanoscale, 2014, 6, 5934
    DOI: 10.1039/C4NR01214C

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