Surface stabilization for enhancing air/moisture resistance of layered Ni-rich oxide cathodes

Layered Ni-rich oxides (LiNi x Co y Mn z O 2 , with x ≥ 0.8 and x + y + z = 1) are promising cathode materials for high-energy-density lithium-ion batteries (LIBs) owing to their high specific capacity and high operating voltage. However, the Ni-rich cathode suffers from notorious deterioration when in contact with ambient air, primarily driven by nickel's multivalent (Ni 2 ⁺/Ni 3 ⁺/Ni 4 ⁺) reactions and humidity sensitivity. In this study, we report a novel surface modification strategy for LiNi 0.83 Co 0.12 Mn 0.05 O 2 (NCM83) via Li x SiO y coating, achieved through chemical grafting using the silane coupling agent, (3-aminopropyl) triethoxysilane (KH550), followed by thermal treatment. The modified NCM83 exhibits enhanced moisture resistance due to a superhydrophobic surface that suppresses detrimental reactions between residual lithium species (Li 2 O, LiOH, etc.) and water. Furthermore, the Li x SiO y coating mitigates mechanical degradation by facilitating strain relaxation. Notably, the modified NCM83 retains high electrochemical performance after 28 days of air exposure, delivering a specific capacity of 157 mAh g⁻ 1 after 100 cycles at 1C, compared to 108 mAh g⁻ 1 for the uncoated counterpart. Overall, these findings present an effective strategy for improving upon the surface stability of Ni-rich cathodes, facilitating their processing and paving the way for large-scale applications in high-energy LIBs.