Artificial Bicontinuous Laminate Synergistically Reinforces and Toughens Dilute Graphene Composites

Strength and toughness are usually exclusive in polymer nanocomposites with dispersed nanofillers. This intrinsic conflict has been relieved in a high filler loading range by mimicking the nacre structure of natural selection. However, at the low loading extreme, it still remains a great challenge. Here, we design a bicontinuous lamellar (BCL) structure to synergistically reinforce and toughen nanocomposites in the dilute range of nanofiller below 1 wt %. At a typical loading of 0.3 wt %, the BCL composite of graphene oxide (GO) and poly(vinyl alcohol) (PVA) has an 8200% toughness and a comparably reinforced hardness of the dispersed counterpart, accompanying a 53-fold higher failure elongation that even exceeds that of pure PVA. Theoretical modeling and experimental analyses reveal that the continuous generation of massive crazes of GO layers endows the BCL composite with high toughness and surprising breakage elongation beyond those of pure PVA. The BCL organization is an alternatively optimal structure model to merge the exclusive strength and toughness together for damage-tolerant nanocomposites with a dilute range of nanofillers, other than nacre-like and well-dispersed structure, providing an alternative methodology to fabricate mechanically robust composites.