Developing high-performance materials from existing natural materials is highly desired because of their environmental friendliness and low cost; two-dimensional nanoclay exfoliated from layered silicate minerals is a good building block to construct multilayered macroscopic assemblies for achieving high mechanical and functional properties. Nevertheless, the efforts have been frustrated by insufficient inter-nanosheet stress transfer and nanosheet misalignment caused by capillary force during solution-based spontaneous assembly, degrading the mechanical strength of clay-based materials. Herein, a constrained assembly strategy that is implemented by in-plane stretching a robust water-containing nanoclay network with hydrogen and ionic bonding is developed to adjust the 2D topography of nanosheets within multilayered nanoclay film. In-plane stretching overcomes capillary force during water removal and thus restrains nanosheet conformation transition from nearly flat to wrinkled, leading to a highly aligned multilayered nanostructure with synergistic hydrogen and ionic bonding. It is proved that inter-nanosheet hydrogen and ionic bonding and nanosheet conformation extension generate profound mechanical reinforcement. The tensile strength and modulus of natural nanoclay film reach up to 429.0 MPa and 43.8 GPa and surpass the counterparts fabricated by normal spontaneous assembly. Additionally, improved heat insulation function and good nonflammability are shown for the natural nanoclay film and extend its potential for realistic uses.
Keywords: constrained assembly; interfacial bonding; mechanical property; nanoclay; two-dimensional conformation.