Exploring the Potential of Carbonized Nano-Si within G@C@Si Anodes for Lithium-Ion Rechargeable Batteries.

Abstract

This study presents the synthesis, characterization, and electrochemical performance evaluation of carbon@silicon (C@Si) and graphite@carbon@silicon (G@C@Si) nanocomposites as potential anode materials for lithium-ion batteries (LIBs). Employing a combination of mechanical milling and carbonization using citric acid, we developed nanocomposites exhibiting unique core-shell structures, as confirmed by detailed SEM and TEM analysis. The G@C@Si nanocomposite displayed superior electrochemical performance, delivering an initial discharge capacity of 1724 mAh g-1 and a high initial Coulombic efficiency of 87.37%. The nanocomposite demonstrated remarkable cycling durability with a discharge capacity of 1248 mAh g-1 over 200 cycles and an average Coulombic efficiency of 99.1% and high-capacity retention of about 83%. Notably, a high capacity of 1325 mAh g-1 was observed at a high 3C rate, and the electrode showed excellent resilience by rapidly recovering to a discharge capacity of 1637 mAh g-1 when the C rate was reduced back to 0.5C. Electrochemical impedance spectra revealed a reduced charge transfer resistance of approximately 43 Ω in the G@C@Si nanocomposite as compared to that of C@Si (∼56 Ω) and nano-Si (105 Ω), indicating enhanced lithium-ion diffusion due to the integration of graphite. Postcycle electrode analysis revealed excellent structural integrity, with minimized volume changes in both C@Si and G@C@Si. XPS studies revealed a thinner SEI layer formation in the G@C@Si electrode compared to C@Si. The C@Si core-shell formation through the citric acid treatment of nano-Si and integration of graphite by mechanical milling significantly boosts the electrochemical performance of the G@C@Si nanocomposite. These findings suggest that the G@C@Si nanocomposite offers immense potential for utilization in high-capacity and high-efficiency LIBs.