High-energy Ni-rich layered oxide cathode materials such as LiNi_0.8Mn_0.1Co_0.1O₂ (NMC811) suffer from detrimental side reactions and interfacial structural instability when coupled with sulfide solid-state electrolytes in all-solid-state lithium-based batteries. To circumvent this issue, here we propose a gradient coating of the NMC811 particles with lithium oxy-thiophosphate (Li₃P_1+xO₄S_4x). Via atomic layer deposition of Li₃PO₄ and subsequent in situ formation of a gradient Li₃P_1+xO₄S_4x coating, a precise and conformal covering for NMC811 particles is obtained. The tailored surface structure and chemistry of NMC811 hinder the structural degradation associated with the layered-to-spinel transformation in the grain boundaries and effectively stabilize the cathode|solid electrolyte interface during cycling. Indeed, when tested in combination with an indium metal negative electrode and a Li₁₀GeP₂S₁₂ solid electrolyte, the gradient oxy-thiophosphate-coated NCM811-based positive electrode enables the delivery of a specific discharge capacity of 128 mAh/g after almost 250 cycles at 0.178 mA/cm² and 25 °C.

高能富镍层状氧化物正极材料，如 LiNi _0.8 Mn _0.1 Co _0.1 O ₂ (NMC811) 在全固态锂基电池中与硫化物固态电解质结合时会发生有害的副反应和界面结构不稳定. _{为规避此问题，我们在此建议使用硫代磷酸锂 (Li 3} P _1+x O ₄ S _4x )对 NMC811 颗粒进行梯度涂层。通过 Li ₃ PO ₄的原子层沉积和随后原位形成梯度 Li ₃ P _1+x O ₄ S _4x涂层，获得了 NMC811 颗粒的精确和保形覆盖。NMC811 定制的表面结构和化学性质阻碍了与晶界中的层状到尖晶石转变相关的结构退化，并在循环过程中有效地稳定了阴极|固体电解质界面。事实上，当与铟金属负极和 Li ₁₀ GeP ₂ S ₁₂固体电解质组合进行测试时，梯度氧硫代磷酸盐涂层 NCM811 基正极能够在几乎完全放电后提供 128 mAh/g 的比放电容量。在 0.178 mA/cm ²和 25 °C 下进行 250 个循环。