The commercialization of the high energy, lithium, and manganese-rich NCM (LMR-NCM) is impeded by its complex interfacial electrochemical processes, oxygen release, and surface degradation. Here, we introduced t-butyl-dimethylsilyllithium as a single-source precursor for depositing Li_xSi_yO_z with an integrated network of siloxane moieties as an artificial cathode/electrolyte interphase (ACEI) which stabilizes LMR-NCM by mitigating oxygen release, electrolyte degradation and preventing fractures. Using solid-state NMR coupled with dynamic nuclear polarization, detailed molecular-level characterization of the ACEI is presented. The proposed CEI enabled improved energy-density at high rates (644 Wh.kg^-1, compared to uncoated material with 457 Wh.kg^-1 at 4C) with suppressed parasitic reactions and O₂ evolution. The efficacy of the CEI is demonstrated in full graphite/LMR-NCM pouch cells with ~ 35% enhanced capacity and >80% capacity retention over 200 cycles. Altogether, these results present the importance of careful selection and design of surface chemistry for stabilizing the electrode/electrolyte interphase in challenging battery chemistries.

高能量，富含锂和锰的NCM（LMR-NCM）的商业化受到其复杂的界面电化学过程，氧气释放和表面降解的阻碍。在这里，我们引入了叔丁基-二甲基甲硅烷基锂作为单源前驱体，用于沉积具有硅氧烷部分集成网络的Li _x Si _y O _z作为人工阴极/电解质中间相（ACEI），可通过减轻氧气释放来稳定LMR-NCM，电解质降解并防止破裂。使用固态核磁共振和动态核极化，ACEI的详细的分子水平表征被提出。拟议的CEI可以提高高密度（644 Wh.kg ^-1的能量密度）与在4C下具有457 Wh.kg ^-1的未涂覆材料相比，具有抑制的寄生反应和O ₂释放。在完整的石墨/ LMR-NCM袋式电池中证明了CEI的功效，在200个循环中，容量提高了35％，容量保持率提高了80％以上。总而言之，这些结果表明了在具有挑战性的电池化学中仔细选择和设计表面化学对于稳定电极/电解质中间相的重要性。