▎ 摘　　要

To take full advantage of graphene in macroscale devices, it is important to integrate two-dimensional graphene nanosheets into a micro/macrosized structure that can fully utilize graphenes nanoscale characteristics. To this end, we developed a novel spray-assisted self-assembly process to create a spherically integrated graphene microstructure (graphene microsphere) using a high-temperature organic solvent in a manner reminiscent of deep-frying. This graphene microsphere improves the electrochemical performance of supercapacitors, in contrast to nonassembled graphene, which is attributed to its structural and pore characteristics. Furthermore, this synthesis method can also produce an effective graphene-based hybrid microsphere structure, in which Si nanoparticles are efficiently entrapped by graphene nanosheets during the assembly process. When used in a Li-ion battery, this material can provide a more suitable framework to buffer the considerable volume change that occurs in Si during electrochemical lithiation/delithiation, thereby improving cycling performance. This simple and versatile self-assembly method is therefore directly relevant to the future design and development of practical graphene-based electrode materials for various energy-storage devices.