Bi-Continuous Si/C Anode Materials Derived from Silica Aerogels for Lithium-Ion Batteries

Poor cycling performance caused by massive volume expansion of silicon (Si) has always hindered the widespread application of silicon-based anode materials. Herein, bi-continuous silicon/carbon (Si/C) anode materials are prepared via magnesiothermic reduction of silica aerogels followed by pitch impregnation and carbonization. To fabricate the expected bi-continuous structure, mesoporous silica aerogel is selected as the raw material for magnesiothermic reduction. It is successfully reduced to mesoporous Si under the protection of NaCl. The as-obtained mesoporous Si is then injected with molten pitch via vacuuming, and the pitch is subsequently converted into carbon at a high temperature. The innovative point of this strategy is the construction of a bi-continuous structure, which features both Si and carbon with a cross-linked structure, which provides an area to accommodate the colossal volume change of Si. The pitch-derived carbon facilitates fast lithium ion transfer, thereby increasing the conductivity of the Si/C anode. It can also diminish direct contact between Si and the electrolyte, minimizing side reactions between them. The obtained bi-continuous Si/C anodes exhibit excellent electrochemical performance with a high initial discharge capacity of 1481.7 mAh g⁻¹ at a current density of 300 mA g⁻¹ and retaining as 813.5 mAh g⁻¹ after 200 cycles and an improved initial Coulombic efficiency of 82%. The as-prepared bi-continuous Si/C anode may have great potential applications in high-performance lithium-ion batteries.