Pistachio-Inspired Bulk Graphene Oxide-Based Materials with Shapeability and Recyclability

Nowadays, despite the fact that recent progress has been reported to mimic natural structural materials (especially nacre), designing bioinspired ultrastrong composites in a universal, viable, and scalable manner still remains a long-standing challenge. In particular, pistachio shells show high tissue strength attributed to the cellulose sheet laminated microstructures. Compared with nacre, pistachio shells own interlocking mortise-tenon joints in their structure, which offer higher energy dissipation and deformability. Here we present a strategy to produce nanocomposites with pistachio-mimetic structures through repeated kneading of graphene oxide (GO) in a dynamic covalent and supramolecular poly(sodium thioctic) (pST) system. The dynamic nature of the polymeric backbones endows the resultant GO-based composite with full recyclability and three-dimensional shapeability. The superior mechanical properties of the pistachio-mimetic composite can be attributed to the mortise-tenon joints design in the structure, which has not been achieved in the nacre-mimetic composite. The resulting composite also exhibits high thermal conductivity (15.6 W/(m·K)), yielding an alternative approach to design in engineered and thermal management materials.