Stabilizing Lini0.8co0.1mn0.1o2 Cathode by Combined Moisture and Hf Digestion/Adsorption for High-Performance Lithium Metal Batteries

Nickel-rich layered oxide cathodes such as LiNi0.8Co0.1Mn0.1O2 are promising to significantly increase the energy density of lithium metal batteries beyond 350 Wh kg-1. However, serious issues regarding cycle stability still remain when matching with conventional non-aqueous carbonate electrolytes that contain fluorine such as lithium hexafluorophosphate (LiPF6). Hydrolysis of LiPF6 generates corrosive hydrofluoric acid (HF), which destroys the cathode structure and accelerates the cathodic dissolution/anodic deposition of transition metal (TM) ions. Here, we demonstrate that ball milling NCM811 with carbon-coated aluminum nitride (AlN-C) remarkably enhances the capacity retention. AlN-C acts both as a scavenger and as an adsorption center to digest and adsorb H2O and HF, respectively. Thereby, it prevents the dissolution of TM ions, which would result in capacity decay and damage to the lithium metal anode. It is demonstrated that the addition of 10 % AlN-C via wet ball milling with NCM811 enables achieving a capacity retention of 88.3 % for the cathode after 200 cycles at 1 C even in a high moisture electrolyte containing 0.1 wt.% H2O. Therefore, this work shows up a pathway to a rational enhancement of the capacity retention and cycle life of nickel-rich cathodes.