Si-on-Graphite fabricated by fluidized bed process for high-capacity anodes of Li-ion batteries

Composites consisting of graphite and silicon have been considered as potential high-capacity anode materials for the next-generation Li-ion batteries (LIBs). The synthesis method is critical for determining the microstructure, which is directly related to the material performance and the cost-efficiency for making commercial electrode materials. Herein, we report the fabrication of silicon-on-graphite (Si@Gr) composites by fluidized bed granulation (FBG) for the first time. The FBG process is shown to produce composite powders comprising a uniform layer of nano-sized Si particles lodged onto the surface of micron-sized graphite particles to possess a core-shell microstructure. Adopting a suitable binder during the FBG process enables a firm adhesion of the Si nanoparticles on graphite surface during subsequent carbon-coating, where the composite particles are coated with pitch and then carbonised to form a highly electronically conductive and mechanical stabilizing layer of amorphous carbon. These carbon-coated composites exhibit a high capacity reaching over 600 mAh g(-1), high rate capability and illustrates the potential of long-cycle stability in Si@Gr parallel to Li metal cells, showing more than 70% capacity retention after 400 charge-discharge cycles even without electrolyte optimization. Furthermore, a significantly improved cycling stability is found for the carbon-coated Si@Gr materials in LiNi0.6Co0.2Mn0.2O2 (NCM-622) parallel to Si@Gr full-cells.

Automated summary

The study reports the fabrication of silicon-on-graphite composites using fluidized bed granulation for the first time, showing the formation of core-shell microstructure. By using a suitable binder during the process, the carbon-coated composites exhibit high capacity, high rate capability, and long cycle stability.