Effect of Short-Chain Polymer Binders on the Mechanical and Electrochemical Performance of Silicon Anodes

Polymer binders are crucial components in providing both mechanical support and chemical stability to the structure of porous Li-ion electrodes. Particularly in silicon anodes, the active material undergoes substantial volume expansion of up to 275%. Due to the mechanical constraint of the current collector, these silicon materials tend to expand in the normal direction while exhibiting substantial particle rearrangement and plastic deformation. Conventional rigid binders such as polyacrylic acid (PAA) and polyimide (PI), while providing satisfactory initial capacity, do not eliminate diminished long-term performance. Our research attempts to develop binder formulations that can accommodate sufficient flexibility for the substantial volume changes of silicon particles. Specifically, we explore the use of short-chain polymer binders and a strategic blend of binders with different molecular weights. Experiments have demonstrated that cells combining both long- and short-chain PAA binders delivered an initial capacity of 2200 mAh/g at a 0.1C rate, compared to 1700 mAh/g for pristine PAA cells. Initial work indicated that shorter polymer chains might compromise the adhesion to the current collector, so we developed a multilayer anode (MLA) structure to mitigate this issue. Nevertheless, at this early stage of development, there was no observed increase in cycling performance for the MLA electrodes.