Efficient Fabrication of High-Capacity Silicon Composite Anodes for All-Solid-State Lithium-Ion Batteries

Silicon is a promising anode material for all-solid-state Li-ion batteries (ASSLIBs), due to its high capacity; however, it suffers from considerable volume expansion (>300%) during cycling, resulting in poor capacity retention, low areal capacities, and low rate capabilities. To address these issues, we propose a μSi/SWCNT/LPSCl composite that effectively coats micrometer-sized Si (μSi) particles with Li₆PS₅Cl and single-walled carbon nanotubes (SWCNTs). This composite improved electrical and ionic conductivities, suppressed interface decomposition between μSi and the Li₆PS₅Cl solid electrolyte during cycling, and mitigated volume expansion to prevent cracks and contact loss. The μSi/SWCNT/LPSCl anode shows a high initial capacity (2974 mAh g^–1 at a 0.1 C rate) and stable retention for 400 cycles. Furthermore, a full cell with this anode and a LiNi_0.8Co_0.1Mn_0.1O₂ cathode exhibited excellent reversibility and stable cycling performance. We anticipate this study will provide a solution for high-performance Si-based anodes in ASSLIBs.