LiPAA binder was prepared by titrating PAA in water with saturated LiOH (aq), creating an 8.5% LiPAA solution at pH ≈ 7.2. Slurries were prepared in an ambient atmosphere by combining as-purchased Si nanoparticles, Super-P and LiPAA in a 60:20:20 ratio and diluting with water (~160% mass of slurry). The solution was mixed in a planetary ball mill (Changsha Tianchuang Powder Technology Co.) at 500 rpm for 60 minutes total in a polyurethane vial using zirconia balls (~500% mass of slurry). The slurry was cast onto copper foil (battery grade, 10 µm) at a cast height of 100 µm and dried overnight at 120 °C under vacuum. Discs were punched with a diameter of 15 mm, then dried again at 120 °C under vacuum for 16 hours and brought directly under inert atmosphere.