Design of layered-stacking graphene assemblies as advanced electrodes for supercapacitors

Graphene is a competitive electrode material for supercapacitors due to its unique two-dimensional structure,large surface area,high conductivity,and good physicochemical stability.However,random agglomeration and restacking of graphene sheets result in a reduced surface area and a loose structure with low density,which severely restricts the application for high gravimetric/volumetric energy density devices.Rational design of the layered-stacking structure of graphene assemblies can effectively prevent the restacking of graphene sheets,construct efficient ion transport channels,and improve spatial utilization,demonstrating the huge potential for developing advanced electrode materials.Herein,from the aspect of improving the electrochemical kinetics through designing efficient electron and ion transport paths,we first highlight the advantages of layered-stacking graphene assemblies,describe some common routes for preparing graphene building units,and then summarize the novel methods to design layered-stacking structures.A comprehensive review of the typical structure including nanocarbon pillared graphene,porous graphene blocks,and graphene ribbon films is provided with a focus on the mechanisms behind the performance improvements.Finally,critical challenges and some general ideas for future development are proposed,which may open up new opportunities for material chemistry and device innovation.