La₄NiLiO₈-Shielded Layered Cathode Materials for Emerging High-Performance Safe Batteries

Low theoretical capacities of the commercial cathode materials (olivine: ∼170 mA h g^-1 and spinel: ∼140 mA h g^-1) dictate the need for higher energy density alternates such as nickel-rich (denotes as NCM) materials with a theoretical capacity of ∼270 mA h g^-1. However, low conductivity and the bulk degradation after direct contact with liquid electrolytes, especially at temperatures higher than 50 °C, are the biggest issues to resolve for safe use and confident commercialization of the NCM materials. In this context, we first report "La₄NiLiO₈ shields" to simultaneously boost charge conduction characteristics and circumvent the electrolytic degradation of NCM. Consequently, the La₄NiLiO₈-shielded LiNi_0.5Co_0.2Mn_0.3O₂ (LSN5) not only offers a 4.1× less charge transfer resistance and significantly higher discharge capacity (219.7 mA h g^-1) than the nonshielded NCM (187 mA h g^-1) and theoretical capacities of commercial cathode materials but also maintains more than 91.7% of capacity retention at 25 °C after 500 cycles and 84.2% at 60 °C after 200 cycles. In contrast, the nonshielded NCM cathodes can only provide 58.9 and 45.5% capacity retentions at corresponding test temperatures and performance cycles. The acquired excellent electrochemical performance and battery stability at both the ambient and high-temperature conductions infer great importance of the novel La₄NiLiO₈ shields in developing high-performance safe secondary batteries.