Constructing a High-Energy and Durable Single-Crystal NCM811 Cathode for All-Solid-State Batteries by a Surface Engineering Strategy

Single-crystal LiNi_0.8Co_0.1Mn_0.1O₂ (S-NCM811) with an electrochemomechanically compliant microstructure has attracted great attention in all-solid-state batteries (ASSBs) for its superior electrochemical performance compared to the polycrystalline counterpart. However, the undesired side reactions on the cathode/solid-state electrolyte (SSE) interface causes inferior capacity and rate capability than lithium-ion batteries, limiting the practical application of S-NCM811 in the ASSB technology. Herein, it shows that S-NCM811 delivers a high capacity (205 mAh g^–1, 0.1C) with outstanding rate capability (175 mAh g^–1 at 0.3C and 116 mAh g^–1 at 1C) in ASSBs by the coating of a nano-lithium niobium oxide (LNO) layer via the atomic layer deposition technique combined with optimized post-annealing treatment. The working mechanism is verified as the nano-LNO layer effectively suppresses the decomposition of sulfide SSE and stabilizes the cathode/SSE interface. The post-annealing of the LNO layer at 400 °C improves the coating uniformity, eliminates the residual lithium salts, and leads to small impedance increasing and less electrochemical polarization during cycling compared with pristine materials. This work highlights the critical role of the post-annealed nano-LNO layer in the applications of a high-nickel cathode and offers some new insights into the designing of high-performance cathode materials for ASSBs.