Supramolecular transparent plastic engineering covalent-and-supramolecular polymerization.

Supramolecular glass and plastic are a new generation of artificial transparent materials that exhibit excellent optical behavior and processability. However, owing to inherent deficiencies in their mechanical toughness and long-term stability, supramolecular materials lack the potential for functionalization and application. Inspired by the toughening phenomena in biological systems, a synergistic covalent-and-supramolecular polymerization strategy was applied to construct plastic-like supramolecular materials with high transmittance the solvent-free one-pot amidation of thioctic acid and (poly)amines. Covalent amide linkers, dynamic disulfide bonds, and hydrogen bonds significantly enhance the mechanical toughness and hardness of supramolecular plastic. Greatly benefitting from covalent-and-supramolecular polymerization, not only does the supramolecular plastic exhibit a high mechanical strength of 45.51 MPa and a rigidity of 74.0 HD, but it is also highly resistant to mechanical impact (34.47 kJ m). Experimental and theoretical investigations demonstrated that polymeric structures connected amide units are responsible for the tough mechanical properties, whereas the dynamic and reversible bonding/debonding of disulfide and hydrogen bonds favor energy dissipation, which together convert supramolecular transparent plastic into a rigid and tough material.