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Abstract Silicon (Si) holds immense promise as viable anode for next‐generation high‐energy‐density Li‐ion batteries (LIBs). However, its poor ionic/electronic conductivity and significant volumetric changes during cycling lead to rapidly deteriorated LIB performance. Here, a novel multifunctional coating featuring ultrafine SiO 2 nanoparticles (<7 nm) embedded carbon on Si nanoparticles (termed Si@uSiO 2 ‐C) to resolve these challenges is proposed. This unique uSiO 2 ‐C coating provides high‐efficient electron and ion transport pathways, while also improves interfacial stability and mitigates volume changes during cycling, thereby enhancing the conductivity and structural integrity of Si@uSiO 2 ‐C, as corroborated by extensive experimental and computational studies. In addition, the abundant interfaces in uSiO 2 ‐C coating facilitate Li + transport and the evenly distributed ultrafine SiO 2 nanoparticles impart high electrochemical reactivity and mechanical robustness. Consequently, the Si@uSiO 2 ‐C anode achieves a high reversible capacity of 2093 mAh g −1 at 0.2 A g −1 , with a high initial Coulombic efficiency of 88.3%, superior rate capability and durability (1000 cycles, 928 mAh g −1 at 1.0 A g −1 , 75% capacity retention). Full cells paired with commercial LiFePO 4 cathodes demonstrate high cyclability, maintaining 80% capacity retention over 500 cycles at 4 C. This work highlights the vital role of multifunctional coating in promoting the electrochemical performance of Si‐based anodes for high‐performance LIBs.
Sun et al. (Mon,) studied this question.