Self-Healable, Tough, and Ultrastretchable Nanocomposite Hydrogels Based on Reversible Polyacrylamide/Montmorillonite Adsorption

Nanocomposite hydrogels with unprecedented stretchability, toughness, and self-healing have been developed by in situ polymerization of acrylamide with the presence of exfoliated montmorillonite (MMT) layers as noncovalent cross-linkers. The exfoliated MMT clay nanoplatelets with high aspect ratios, as confirmed by transmission electron microscopy (TEM) and X-ray diffraction (XRD) results, are well dispersed in the polyacrylamide matrix. Strong polymer/MMT interaction was confirmed by Fourier transform infrared spectroscopy (FTIR) and differential scanning calorimetry (DSC). The effective cross-link densities of these hydrogels are estimated in the range of 2.2-5.7 mol m(-3). Uniaxial tensile tests showed a very high fracture elongation up to 11 800% and a fracture toughness up to 10.1 MJ m(-3). Cyclic loading-unloading tests showed remarkable hysteresis, which indicates energy dissipation upon deformation. Residual strain after cyclic loadings could be recovered under mild conditions, with the recovery extent depending on clay content. A mechanism based on reversible desorption/adsorption of polymer chains on clay platelets surface is discussed. Finally, these nanocomposite hydrogels are demonstrated to fully heal by dry-reswell treatments.