Dendrimer Based Binders Enable Stable Operation of Silicon Microparticle Anodes in Lithium‐Ion Batteries

High-capacity anode materials (e.g., Si) are highly needed for high energy density battery systems, but they usually suffer from low initial coulombic efficiency (CE), short cycle life, and low-rate capability caused by large volume changes during the charge and discharge process. Here, a novel dendrimer-based binder for boosting the electrochemical performance of Si anodes is developed. The polyamidoamine (PMM) dendrimer not only can be used as binder, but also can be utilized as a crosslinker to construct 3D polyacrylic acid (PAA)-PMM composite binder for high-performance Si microparticles anodes. Benefiting from maximum interface interaction, strong average peeling force, and high elastic recovery rate of PAA-PMM composite, the Si electrode based on PAA-PMM achieves a high specific capacity of 3590 mAh g-1 with an initial CE of 91.12%, long-term cycle stability with 69.80% retention over 200 cycles, and outstanding rate capability (1534.8 mAh g-1 at 3000 mA g-1 ). This work opens a new avenue to use dendrimer chemistry for the development of high-performance binders for high-capacity anode materials.