The key issue in utilizing solid polymer electrolytes for high-energy-density lithium metal batteries is to balance the conflicting demands of superior processability, adequate ionic conductivity, and mechanical stability. Inspired by molecular structure design, a metal-organic framework-derived polyether poly(urethane urea) solid polymer electrolyte (denoted as ePU@H SPE) has been synthesized via a facile polycondensation method involving covalent crosslinking. The reduced crystallinity and numerous polar groups in ePU@H SPEs enhance Li salt dissociation and create efficient Li⁺ ion diffusion channels, yielding remarkable ionic conductivity (1.48 × 10⁻⁴ S cm⁻¹). The polymer backbones, incorporating covalent bonds and dynamic hydrogen bonds, provide superb mechanical strength (5.12 GPa), high toughness (1240%), and excellent resilience, which suppress lithium dendrite growth and buffer electrode volume fluctuations during cycling. Leveraging these attributes, the well-designed ePU@H SPE enables ultra-high durability in lithium plating/stripping over 2300 h. Moreover, the integrated LFP|ePU@H|Li batteries, generating delicate electrode/electrolyte interfacial contact, deliver an exceptionally long lifespan (86% retention over 500 cycles at 1 C). Moreover, the LFP|ePU@H|Li pouch cell operates reliably even under severe deformation and external damage. Impressively, the stable cycling performance of full batteries incorporating high-voltage LCO and high-capacity S cathodes further verifies the significant potential of advanced ePU@H SPEs for practical applications.

中文翻译：

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通过共价交联实现金属有机框架衍生的弹性固体聚合物电解质，用于高性能锂金属电池


将固体聚合物电解质用于高能量密度锂金属电池的关键问题是平衡卓越的可加工性、足够的离子导电性和机械稳定性的冲突需求。受分子结构设计的启发，通过涉及共价交联的简单缩聚方法合成了一种金属有机框架衍生的聚醚聚（氨基甲酸酯脲）固体聚合物电解质（表示为 ePU@H SPE）。ePU@H SPE 中结晶度降低和极性基团多，增强了 Li盐解离并产生高效的 Li⁺ 离子扩散通道，从而产生显著的离子电导率 （1.48 × 10⁻⁴ S cm⁻¹）。聚合物主链包含共价键和动态氢键，具有出色的机械强度 （5.12 GPa）、高韧性 （1240%） 和出色的弹性，可抑制锂枝晶生长和循环过程中缓冲电极体积波动。利用这些特性，精心设计的 ePU@H SPE 可在 2300 小时内实现超高的锂电镀/剥离耐久性。此外，集成的 LFP|ePU@H|锂电池产生精细的电极/电解质界面接触，具有极长的使用寿命（在 1 C 下循环 500 次后保持 86%）。此外，LFP|ePU@H|Li 软包电池即使在严重变形和外部损坏的情况下也能可靠运行。令人印象深刻的是，包含高压 LCO 和高容量 S 阴极的满电池的稳定循环性能进一步验证了先进 ePU@H SPE 在实际应用中的巨大潜力。