Impact of Binder Content and Type on the Electrochemical Performance of Silicon Anode Materials

Binders are crucial for stabilizing the cycling performance of silicon (Si) materials by preventing Si particle pulverization during lithiation and delithiation. Poly(acrylic acid) (PAA) and carboxymethyl cellulose (CMC) are the two most studied binders for Si electrodes, with PAA being an elastic polymer and CMC a rigid polymer. Starting with the elastic PAA, in this work the impact of binder content on the cycling performance of Si electrodes is studied. It is found that regardless of Si particle size, there is an optimal binder content between 20 % and 25 % for the cycling stability of Si electrodes. On the other hand, the rigid CMC binder results in lower capacity and faster capacity fading for Si electrodes compared with the elastic PAA. AC-impedance analysis reveals that the lower capacity is due to higher grain boundary resistance (R_gb) in CMC-coated electrodes, leading to high charge-transfer resistance (R_ct) and increased polarization. This high polarization triggers premature termination during the discharging process (i. e., the lithiation) of Li/Si cells, underutilizing the Si active material. Additionally, the rapid capacity fading of CMC-coated electrodes is attributed to the rigid binder's inferior ability to prevent Si particle pulverization.