One-step fabrication of binder-free nanoSi-CNT-carbon black/cyclized PAN composite anode for high-performance lithium-ion batteries

Silicon is one of the most promising anode materials for lithium-ion batteries (LIBs) due to its high theoretical capacity. However, its non-conductive nature and significant volume expansion during lithiation pose challenges. In this study, we developed a novel electrode comprising silicon nanoparticles (nanoSi), carbon nanotubes (CNTs), and carbon black (CB) in cyclized polyacrylonitrile (cPAN), referred to as nanoSi-CNT-CB/cPAN. This electrode is fabricated through a one-step thermal process by heating a cast nanoSi-CNT-CB/PAN film on Cu foil at 310 °C. The LIB performance using the nanoSi-CNT-CB/cPAN electrode shows an impressive initial coulombic efficiency of 93.1 % at 0.1 A g, a high specific capacity of 2267.2 mAh g at 0.5 A g, and a retention of 89.2 % over 390 cycles, achieving 783 mAh g at 5 A g. We attribute these results to the fused cPAN, which provides good adhesion to nanoSi, CNTs, CB, and Cu foil, acting as a binder, active material, and ionic conductive medium. The well-dispersed CNTs and CB form an effective conductive network in the electrode. Additionally, the one-step electrode fabrication is a simple and cost-effective process for next-generation Si-based LIBs.