Practical Approach to Enhance Compatibility in Silicon/Graphite Composites to Enable High-Capacity Li-Ion Battery Anodes

[Image: see text] There is an urgent need to improve the energy density of Li-ion batteries to enable mass-market penetration of electric vehicles, grid-scale energy storage, and next-generation consumer electronics. Silicon–graphite composites are currently the most plausible anode material to overcome the capacity limit of graphite or poor cycling performance of silicon. One serious and unrecognized limitation to the use of the composite as an anode is the incompatibility of hydrophobic (natural) graphite with the hydrophilic Si, which adversely affects battery performance. Herein, we report a novel, practical approach to modify the graphite resulting in the formation of a hard carbon coating and graphene sheets that give rise to higher compatibility with Si nanoparticles in the composite. Electrochemical and battery testing of the composite (10 wt % Si) anode shows higher reversible capacity (10% at C/12 and 20% at C/2) than the composite with unmodified graphite reaching ∼600 mAh/g with 95% retention after 100 cycles. The enhanced battery performance is explained by the uniform distribution of Si nanoparticles at the modified graphite surface due to the presence of graphene conductive networks and a thin, oxygen-rich, amorphous carbon layer on the surface of graphite particles, as evidenced by transmission electron microscopy (TEM) images and X-ray photoelectron spectra (XPS). This work provides a new approach to prepare graphite compatible materials that can work with hydrophilic components other than silicon for various applications other than batteries.