Stacking order reduction in multilayer graphene by inserting nanospacers

Toward macroscopic applications of graphene, it is desirable to preserve the superior properties of single-layer graphene in bulk scale. However, the AB-stacking structure is thermodynamically favored for multilayer graphene and causes strong interlayer interactions, resulting in property degradation. A promising approach to prevent the strong interlayer interaction is the staking order reduction of graphene, where the graphene layers are rotated in-plane to form a randomly stacking structure. In this study, we propose a strategy to effectively decrease the stacking order of multilayer graphene by incorporating nanospacers, cellulose nanofibers, or nano-diamonds (NDs) in the formation process of porous graphene sponges. We conducted an ultrahigh temperature treatment at 1500 °C with ethanol vapor for the reduction and structural repair of graphene oxide sponges with different concentrations of the nanospacers. Raman spectroscopy indicated an obvious increase in the random-stacking fraction of graphene by adding the nanospacers. The x-ray diffraction (XRD) analysis revealed that a small amount of the nanospacers induced a remarkable decrease in ordered graphene crystalline size in the stacking direction. It was also confirmed that a layer-number increase during the thermal treatment was suppressed by the nanospacers. The increase in the random-stacking fraction is attributed to the efficient formation of randomly rotated graphene through the ethanol-mediated structural restoration of relatively thin layers induced by the nanospacers. This stacking-order-reduced graphene with bulk scale is expected to be used in macroscopic applications, such as electrode materials and wearable devices.