Single-ion conducting polymer electrolytes, characterized by effective Li⁺ transport and dendrite mitigation, are emerging as promising candidates for the highly demanded lithium metal batteries. However, despite the promise, their current ionic conductivity and Li⁺ transference number fall short of application requirements. Herein, we have developed a free-standing single-ion conducting semi-solid polymer electrolyte (PBSIL), engineered through the synergistic interaction between anion acceptors and solvated ionic liquids. This innovative chemical synergy significantly enhances the complete dissociation of lithium salts while immobilizing anions, thus facilitating rapid Li⁺ transport. As a result, the PBSIL electrolyte exhibits enhanced ionic conductivity of 8.0 × 10⁻⁴ S cm⁻¹, and an improved Li⁺ transference number of 0.75. These features effectively mitigate concentration polarization and dendrite growth, ensuring long-term cell stability. Moreover, Li|PBSIL|LiNi_0.8Co_0.1Mn_0.1O₂ cells demonstrate an ultra-long cycle life of 1300 cycles, with a high discharge capacity of 183 mA h g⁻¹ and excellent capacity retention of 75%. Additionally, PBSIL has been successfully integrated for the first time into the production of winding-processed semi-solid state cylindrical and Z-stacked pouch lithium metal batteries. Through the synergistic regulation of Li⁺ transport and anion immobilization, PBSIL provides an effective design strategy for free-standing semi-solid polymer electrolytes, showcasing superior electrochemical performance and contributing to the development and industrialization of long-cycling lithium metal batteries.

中文翻译：

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一种用于高性能实用锂金属电池的一体化独立式单离子导电半固体聚合物电解质


单离子导电聚合物电解质具有有效的Li ⁺传输和枝晶抑制的特点，正在成为高需求的锂金属电池的有希望的候选者。然而，尽管有这样的前景，但它们目前的离子电导率和Li ⁺迁移数仍达不到应用要求。在此，我们开发了一种独立式单离子导电半固体聚合物电解质（PBSIL），通过阴离子受体和溶剂化离子液体之间的协同相互作用进行设计。这种创新的化学协同作用显着增强了锂盐的完全解离，同时固定阴离子，从而促进快速Li ⁺传输。结果，PBSIL电解质表现出8.0×10 ^-4 S cm ^-1的增强的离子电导率和0.75的改善的Li ⁺迁移数。这些特性有效地减轻了浓差极化和枝晶生长，确保了电池的长期稳定性。此外，Li|PBSIL|LiNi _0.8 Co _0.1 Mn _0.1 O ₂电池表现出1300次循环的超长循环寿命，具有183 mA hg ^-1的高放电容量和75%的优异容量保持率。此外，PBSIL 已首次成功集成到卷绕加工的半固态圆柱形和Z形堆叠软包锂金属电池的生产中。 通过Li ⁺传输和阴离子固定的协同调控，PBSIL为独立式半固体聚合物电解质提供了有效的设计策略，展示了优异的电化学性能，为长循环锂金属电池的开发和产业化做出了贡献。