Stable Silicon Anode for Lithium-Ion Batteries through Covalent Bond Formation with a Binder via Esterification

Silicon (Si) is considered to be one of the most promising anode candidates for next-generation lithium-ion batteries because of its high theoretical specific capacity and low discharge potential. However, its poor cyclability, caused by tremendous volume change during cycling, prevents commercial use of the Si anode. Herein, we demonstrate a high-performance Si anode produced via covalent bond formation between a commercially available Si nanopowder and a linear polymeric binder through an esterification reaction. For efficient ester bonding, polyacrylic acid, composed of -COOH groups, is selected as the binder, Si is treated with piranha solution to produce abundant -OH groups on its surface, and sodium hypophosphite is employed as a catalyst. The as-fabricated electrode exhibits excellent high rate capability and long cycle stability, delivering a high capacity of 1500 mA h g^-1 after 500 cycles at a high current density of 1000 mA g^-1 by effectively restraining the susceptible sliding of the binder, stabilizing the solid electrolyte interface layer, preventing the electrode delamination, and suppressing the Si aggregation. Furthermore, a full cell is fabricated with as-fabricated Si as an anode and commercially available LiNi_0.6Mn_0.2Co_0.2O₂ as a cathode, and its electrochemical properties are investigated for the possibility of practical use.