Advanced anodes composed of graphene encapsulated nano-silicon in a carbon nanotube network

High-capacity silicon-based anode materials with high conductivity to promote electron/ion transfer and excellent elasticity to alleviate volume expansion during repeated lithiation/delithiation process are highly desirable for next-generation lithium-ion batteries. Herein, we developed a facile in situ synthesis method based on chemical vapor deposition to fabricate Si-based nanocomposites integrated with interlinked graphene (Gra) and carbon nanotube (CNT). With melt-assembly nanosized Cu as the catalyst, hierarchical three-dimensional conductive Gra/CNT networks were in situ grown onto Si nanoparticles (SNPs) to achieve the Si@Gra@CNT composite. Such a hierarchical structure combines multiple advantages from SNPs with a super high capacity, Gra/CNT framework with continuous electrical conductivity, and void space for tolerance of Si volume expansion. Moreover, the SNPs were conformally encapsulated by few-layer Gra (fGra), which can protect the SNPs from direct exposure to electrolyte, resulting in a stable solid-electrolyte interface. As an anode material for Li-ion battery, the as-prepared Si@Gra@CNT composite exhibited a high initial specific capacity of 1197 mA h g(-1) at a current density 2.0 A g(-1) and similar to 82% capacity retention over 1200 cycles, which was much better than those of Si@Gra and Si@CNT composites. The mechanism for the improved electrochemical performance was further analysed from the aspect of the synergetic effect arising from the construction components.