Biological
tissues, such as heart valve, tendon, etc.,
possess
excellent mechanical properties, which arises from their inherent
anisotropic arrangement of soft and hard phases. Inspired by the anisotropic
structures, many methods have been developed to synthesize hydrogels
that can achieve mechanical properties comparable to biological tissues.
Here, we describe a new method to enhance fracture toughness and fatigue
resistance of hydrogels by introducing nanofibers which can reversibly
align with elastic deformation to form an anisotropic structure. As
a demonstration, we introduce stiff, rod-like cellulose nanocrystals
(CNCs) into a polyacrylamide (PAAm) network. CNCs aggregate into clusters
to form hard phases and entangle with the PAAm network. The CNC/PAAm
composite hydrogel is initially isotropic, becomes anisotropic upon
loading, and recovers to be isotropic upon unloading. During the deformation,
the aligned CNC clusters at the crack tip can transmit the stress
over the size of the cluster, effectively resisting crack growth.
We use photoelasticity and small-angle X-ray scattering (SAXS) tests
to observe the change of microstructures associated with deformation.
The fracture toughness of CNC/PAAm hydrogels with different sizes
of CNCs can reach 1000 J/m2. The fatigue threshold is about
100 J/m2, an order of magnitude higher than that of PAAm
hydrogel. This work provides a simple and general method to strengthen
hydrogels under both monotonic and cyclic loads.