Shear‐Induced Interfacial Structural Conversion of Graphene Oxide to Graphene at Macroscale

Abstract The controllable adjustment of an ideal graphene structure on the surface/interface is important to achieve many of the potential characteristics and applications of graphene. Here, a phenomenon is observed in which friction can induce the structural conversion of graphene oxide (GO) to graphene perfectly on a macroscale sliding interface. The controlling factors and molecular interaction mechanism are further revealed by experiments and theoretical simulation. The results show that shear force drives the tribochemical reactions between the –OH group of GO and active bond of the counterpart, as well as the –OH groups of adjacent GO sheets, leading to the breakage of the COH bond. This leads to the transformation of the sp³ C to sp² C, thereby forming a perfect six‐membered ring. The as‐broken hydroxyl groups combine with the dangling bond of the frictional pair or capture hydrogen from the hydroxyl group of the adjacent GO sheet and generate water molecules. This study provides more information on a novel method of manipulating the interfacial structure of graphene at a macroscale by a simple sliding action. The method also provides a new way of force sensing through the detection of the released H₂O molecules.