Constructing a Low-Cost Si-NSs@C/NG Composite by a Ball Milling-Catalytic Pyrolysis Method for Lithium Storage

Silicon-based composites are promising candidates as the next-generation anode materials for high-performance lithium-ion batteries (LIBs) due to their high theoretical specific capacity, abundant reserves, and reliable security. However, expensive raw materials and complicated preparation processes give silicon carbon anode a high price and poor batch stability, which become a stumbling block to its large-scale practical application. In this work, a novel ball milling-catalytic pyrolysis method is developed to fabricate a silicon nanosheet@amorphous carbon/N-doped graphene (Si-NSs@C/NG) composite with cheap high-purity micron-size silica powder and melamine as raw materials. Through systematic characterizations such as XRD, Raman, SEM, TEM and XPS, the formation process of NG and a Si-NSs@C/NG composite is graphically demonstrated. Si-NSs@C is uniformly intercalated between NG nanosheets, and these two kinds of two-dimensional (2D) materials are combined in a surface-to-surface manner, which immensely buffers the stress changes caused by volume expansion and contraction of Si-NSs. Attributed to the excellent electrical conductivity of graphene layer and the coating layer, the initial reversible specific capacity of Si-NSs@C/NG is 807.9 mAh g^-1 at 200 mA g^-1, with a capacity retention rate of 81% in 120 cycles, exhibiting great potential for application as an anode material for LIBs. More importantly, the simple and effective process and cheap precursors could greatly reduce the production cost and promote the commercialization of silicon/carbon composites.