A gradient-distributed binder with high energy dissipation for stable silicon anode

Silicon is considered as a promising alternative to traditional graphite anode for lithium-ion batteries. Due to the dramatic volume expansion of silicon anode generated from the insertion of Li⁺ ions, the binder which can suppress the severe volume change and repeated massive stress impact during cycling is required greatly. Herein, we design a gradient-distributed two-component binder (GE-PAA) to achieve excellent cyclic stability, and reveal the mechanism of high energy dissipative binder stabilized silicon electrodes. The inner layer of the electrode is the polyacrylic acid polymer (PAA) with high Young's modulus, which is used as the skeleton binder to stabilize the silicon particle interface and the electrode structure. The outer layer is the gel electrolyte polymer (GE) with lower Young's modulus, which releases the stress generated during the lithiation and de-lithiation process effectively, achieving the high structural stability at the molecular level and silicon particles. Due to the synergistic effect of the gradient binder design, the silicon electrode retains a reversible capacity of 1557.4 mAh g^-1 after 200 cycles at the current density of 0.5 C and 1539.2 mAh g^-1 at a high rate of 1.8 C. This work provides a novel binder design strategy for Si anode with long cycle stability.