Mechanically Reinforced Localized Structure Design to Stabilize Solid–Electrolyte Interface of the Composited Electrode of Si Nanoparticles and TiO₂ Nanotubes

Silicon anode with extremely high theoretical specific capacity (≈4200 mAh g⁻¹), experiences huge volume changes during Li-ion insertion and extraction, causing mechanical fracture of Si particles and the growth of a solid–electrolyte interface (SEI), which results in a rapid capacity fading of Si electrodes. Herein, a mechanically reinforced localized structure is designed for carbon-coated Si nanoparticles (C@Si) via elongated TiO₂ nanotubes networks toward stabilizing Si electrode via alleviating mechanical strain and stabilizing the SEI layer. Benefited from the rational localized structure design, the carbon-coated Si nanoparticles/TiO₂ nanotubes composited electrode (C@Si/TiNT) exhibits an ideal electrode thickness swelling, which is lower than 1% after the first cycle and increases to about 6.6% even after 1600 cycles. While for traditional C@Si/carbon nanotube composited electrode, the initial swelling ratio is about 16.7% and reaches ≈190% after 1600 cycles. As a result, the C@Si/TiNT electrode exhibits an outstanding capacity of 1510 mAh g⁻¹ at 0.1 A g⁻¹ with high rate capability and long-time cycling performance with 95% capacity retention after 1600 cycles. The rational design on mechanically reinforced localized structure for silicon electrode will provide a versatile platform to solve the current bottlenecks for other alloyed-type electrode materials with large volume expansion toward practical applications.