Facile synthesis of core-shell structured Si@graphene balls as a high-performance anode for lithium-ion batteries

Encapsulating silicon (Si) nanoparticles with graphene nanosheets in a microspherical structure is proposed to increase electrical conductivity and solve stability issues when using Si as an anode material in lithium-ion batteries (LIBs). Currently the main strategies to produce high-quality Si-graphene (Si@Gra) electrodes are (1) chemical vapor deposition (CVD) of graphene grown in situ on Si by hydrocarbon precursors and (2) encapsulating Si with a graphene oxide followed by postannealing. However, both methods require a high-temperature and are costly and time-consuming procedures, which hinders their mass scalability and practical utilization. Herein, we report a Si@Gra composite with a ball-like structure that is assembled by a facile spray drying process without a postannealing treatment. The graphene sheets are synthesized by an electrochemical exfoliation method from natural graphite. The resulting Si@Gra composite exhibits a unique core-shell structure, from which the ball-like morphology and the number of graphene layers in the Si@Gra composites are found to affect both the electric conductivity and ionic conductivity. The Si@Gra composites are found to increase the capacity of the anode and provide excellent cycling stability, which is attributed to the high electrical conductivity and mechanical flexibility of the layered graphene; additionally, a void space in the core-shelled ball structure inside the Si@Gra compensates for the Si volume expansion. As a result, the Si@few-layer graphene ball anode exhibits a high initial discharge capacity of 2882.3 mA h g^-1 and a high initial coulombic efficiency of 86.9% at 0.2 A g^-1. The combination of few-layer graphene sheets and the spray drying process can effectively be applied for large-scale production of core-shell structured Si@Gra composites as promising anode materials for use in high-performance LIBs.