Constructing Three-Dimensional Honeycombed Graphene/Silicon Skeletons for High-Performance Li-Ion Batteries

Silicon has been considered to be an attractive high-capacity anode material for next-generation lithium-ion batteries (LIBs). Currently, the commercial application of Si-based anodes is still restricted by its limited cycle life and rate capacity, which could be ascribed to the colossal volumetric change during the cycling process and poor electronic conductivity. We report the design of a unique Si-based nanocomposite of three-dimensional (3D) honeycombed graphene aerogel and the reduced graphene oxide sheets preprotected silicon secondary particles (SiNPs@rGO1). Through simple electrostatic self-assembly and hydrothermal processes, SiNPs are able to be wrapped with rGO1 to form reunited SiNPs@rGO1, and embedded into the backbone of 3D graphene honeycomb (rGO2). Such an intriguing design (namely, SiNPs@rGO1/rGO2) not only provides a conductive skeleton to improve the electrical conductivity, but also possesses abundant void spaces to accommodate the dramatic volume changes of SiNPs. Meanwhile, the outer rGO1 coats protect the inner SiNPs away from the electrolyte and prevent the destruction of the solid electrolyte interphase (SEI) film. As a result, the 3D honeycombed architecture achieves a high cyclability and excellent rate capability.