Despite their enormous potential as a high-energy-density power source, practical applications of Li-metal batteries have been plagued mainly by poor electrochemical longevity. Here, we present an electrode-customized separator (EC separator) based on self-assembled chiral nematic liquid crystalline cellulose nanocrystal (LC–CNC) as a natural material strategy to simultaneously address the electrochemical reversibility issues of both Li-metal anodes and high-capacity cathodes in Li-metal full cells. The EC separator (thickness ∼ 10 μm) comprises a 3-glycidyloxypropyl trimethoxysilane (GPTMS)-modified LC–CNC layer on a polyethylene (PE) separator support layer. The LC–CNC layer enables facile/uniform Li⁺ flux toward Li-metal anodes owing to its ordered nanoporous channels and nanofluidic ion migration effect, thus improving Li plating/stripping cyclability. The GPTMS of the LC–CNC layer chelates heavy metal ions dissolved from high-capacity LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) cathodes, thereby enhancing structural stability of the cathodes. The resulting EC separator enables a Li-metal full cell to improve the volumetric energy density (1016 Wh L_cell⁻¹), cycling retention (84% after 100 cycles vs. 0% for the pristine PE separator), and dimensional stability of the Li-metal anode under constrained cell conditions (thin Li-metal anode (20 μm)/high-capacity NCM811 cathode), which outperform those of previously reported synthetic material-based separators for Li-metal full cells.

尽管锂金属电池具有作为高能量密度电源的巨大潜力，但锂金属电池的实际应用主要受到电化学寿命差的困扰。在这里，我们提出了一种基于自组装手性向列液晶纤维素纳米晶体（LC-CNC）的电极定制隔膜（EC隔膜）作为一种天然材料策略，以同时解决锂金属负极和高-锂金属负极的电化学可逆性问题。锂金属全电池中的容量正极。EC 隔膜（厚度约 10 μm）包含聚乙烯（PE）隔膜支撑层上的 3-缩水甘油氧基丙基三甲氧基硅烷（GPTMS）改性的 LC-CNC 层。LC-CNC 层可实现轻松/均匀的 Li ⁺由于其有序的纳米多孔通道和纳米流体离子迁移效应，通量流向锂金属负极，从而提高了锂电镀/剥离循环性。_{LC-CNC层的GPTMS螯合从高容量LiNi 0.8} Co _0.1 Mn _0.1 O ₂ (NCM811)正极中溶解的重金属离子，从而提高正极的结构稳定性。由此产生的 EC 隔膜使锂金属全电池能够提高体积能量密度（1016 Wh L_电池^-1)、循环保持率（100 次循环后为 84%，而原始 PE 隔膜为 0%）和锂金属负极在受限电池条件下的尺寸稳定性（薄锂金属负极 (20 μm)/高容量 NCM811 正极） )，其性能优于先前报道的用于锂金属全电池的合成材料隔膜。