Evaluating Polyacrylic Acid as a Universal Aqueous Binder for Ni‐Rich Cathodes NMC811 and Si Anodes in Full Cell Lithium‐ion Batteries

Abstract Silicon (Si) and silicon/graphite (Si/Gr) composite anodes are promising candidates due to their high theoretical capacity, low operating potential and natural abundance for high energy density Li‐ion batteries. Green electrode production, eliminating organic volatile solvents require advancement of aqueous electrodes. Engineering the binder plays a critical role for improving waterborne electrodes. Lithium substituted polyacrylic acid LiPAA has been demonstrated as a promising binder for Si/Gr anodes and for Ni‐rich cathodes in different cell configurations. LiPAA is utilized to minimize the volume expansion during cycling for Si/Gr anodes. LiPAA is formed in situ during cathode slurry preparation to regulate the pH and dimmish the Li loss. Using advanced characterization techniques, we investigated the slurries, electrodes, and active material reaction with LiPAA and its effect to the cycling performance. Our results indicate that the performance of high Si containing anode is limited by the amount of Si in the electrode. The failure mechanism with respect to high Si content was studied thoroughly. Aqueous processed cathodes with LiPAA binder in combination with Si anodes outperformed NMP based cathodes. Hence, LiPAA was successfully utilized as an active binder for both a high Si containing anode and for a Ni rich cathode.