Silicon-based anodes are promising to replace graphite-based anodes for high-capacity lithium-ion batteries (LIB). However, the charge-discharge cycling suffers from internal stresses created by large volume changes of silicon, which form silicon-lithium compounds, and excessive consumption of lithium by irreversible formation of lithium-containing compounds. Consumption of lithium by the initial conditioning of the anode, as indicated by low initial coulombic efficiency (ICE), and subsequently continuous formation of solid-electrolyte-phase (SEI) on the freshly exposed silicon surface, are among the main issues. A high-performance, silicon-based, high-capacity anode exhibiting 88.8% ICE and the retention of 2 mAh/cm2 areal capacity after 200 discharge-charge cycles at the rate of 1 A/g is reported. The anode is made on a copper foil using a mixture of 70%:10%:20% by weight ratio of silicon flakes of 100 × 800 × 800 nm in size, Super P conductivity enhancement additive, and an equal-weight mixture of CMC and SBR binders. Pyrolysis of fabricated anodes at 700 °C in argon environment for 1 h was applied to convert the binders into a porous graphitic carbon structure that encapsulates individual silicon flakes. The porous anode has a mechanically strong and electrically conductive graphitic carbon structure formed by the pyrolyzed binders, which protect individual silicon flakes from excessive reactions with the electrolyte and help keep small pieces of broken silicon flakes together within the carbon structure. The selection and amount of conductivity enhancement additives are shown to be critical to the achievement of both high-ICE and high-capacity retention after long cycling. The Super P conductivity enhancement additive exhibits a smaller effective surface area where SEI forms compared to KB, and thus leads to the best combination of both high-ICE and high-capacity retention. A silicon-based anode exhibiting high capacity, high ICE, and a long cycling life has been achieved by the facile and promising one-step fabrication process.
Keywords: Ketjen black; LIB; Super P; anode; initial coulombic efficiency; pyrolysis; retention; silicon.