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

Layered Ni-rich oxides (LiNixCoyMnzO${}_2$, 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. ... mehrOverall, 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.