Abstract

AbstractNickel‐rich cathode materials such as LiNi0.9Co0.05Mn0.05O2 (NMC90) have gained attention due to their ability to deliver high energy densities while being cost‐effective for Lithium‐ion battery manufacturing. However, NMC90 cathodes suffer irreversible parasitic reactions such as electrolyte decomposition, severe capacity fading and impedance build‐up upon prolonged cycling. Herein, we synthesize a conformal ultrathin, surface protection layer on NMC90 powder using ZnxOy via atomic layer deposition technique (ZnxOy@NMC90). Prolonged electrochemical investigation of full cells at high discharge rates of 2 C shows that ZnxOy@NMC90 cells yielded ~31 % improvement in discharge capacity compared to pristine NMC90. Furthermore, operando electrochemical mass spectroscopy studies show that the ZnxOy@NMC90 cells have significantly suppressed electrolyte decomposition as compared to pristine NMC90 cells. Post‐cycling electrochemical impedance spectroscopy studies show that the ZnxOy@NMC90 full cells have significantly reduced impedance compared with pristine NMC90 cells. Additionally, post cycling manganese dissolution studies show that ZnxOy@NMC90 cells have greatly enhanced chemo‐mechanical integrity thereby contributing to improved electrochemical performances. Our results underscore the potential of tailored ZnxOy surface coatings on nickel‐rich cathode materials to address critical challenges in advanced energy storage systems, offering promising prospects for the development of high‐energy‐density lithium‐ion batteries.

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