High-Entropy Microdomain Interlocking Polymer Electrolytes for Advanced All-Solid-State Battery Chemistries,Advanced Materials

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High-Entropy Microdomain Interlocking Polymer Electrolytes for Advanced All-Solid-State Battery Chemistries
Advanced Materials ( IF 27.4 ) Pub Date : 2022-11-07 , DOI: 10.1002/adma.202209402
Yun Su _{1,

2,

3} , Xiaohui Rong _{2,

3,

4} , Hong Li _{2,

3,

4} , Xuejie Huang _{2,

3,

4} , Liquan Chen _{2,

3,

4} , Binyuan Liu _{1,

5} , Yong-Sheng Hu _{2,

3,

4}

Affiliation

All-solid-state polymer electrolytes (ASPEs) with excellent processivity are considered one of the most forward-looking materials for large-scale industrialization. However, the contradiction between improving the mechanical strength and accelerating the ionic migration of ASPEs has always been difficult to reconcile. Herein, a rational concept is raised of high-entropy microdomain interlocking ASPEs (HEMI-ASPEs), inspired by entropic elasticity well-known in polymer and biochemical sciences, by introducing newly designed multifunctional ABC miktoarm star terpolymers into polyethylene oxide for the first time. The tailor-made HEMI-ASPEs possess multifunctional polymer chains, which induce themselves to assemble into micro- and nanoscale dynamic interlocking networks with high topological structure entropy. HEMI-ASPEs achieve excellent toughness, considerable ionic conductivity, an appreciable lithium transference number (0.63), and desirable thermal stability (T_d > 400 °C) for all-solid-state lithium metal batteries. The Li|HEMI-ASPE-Li|Li symmetrical cell shows a stable Li plating/stripping performance over 4000 h, and a LiFePO₄|HEMI-ASPE-Li|Li full cell exhibits a high capacity retention (≈96%) after 300 cycles. This work contributes an innovative design concept introducing high-entropy supramolecular dynamic networks for ASPEs.

中文翻译：

用于高级全固态电池化学的高熵微域互锁聚合物电解质

全固态聚合物电解质（ASPEs）具有优异的加工性能，被认为是最具前瞻性的大规模工业化材料之一。然而，提高机械强度和加速ASPEs的离子迁移之间的矛盾一直难以调和。在此，受高分子和生物化学科学中众所周知的熵弹性的启发，首次将新设计的多功能 ABC 微臂星形三元共聚物引入聚环氧乙烷中，提出了高熵微区互锁 ASPEs (HEMI-ASPEs) 的合理概念。定制的 HEMI-ASPE 具有多功能聚合物链，可诱导自身组装成具有高拓扑结构熵的微米级和纳米级动态互锁网络。HEMI-ASPE 具有出色的韧性，T _d > 400 °C) 对于全固态锂金属电池。Li|HEMI-ASPE-Li|Li 对称电池在 4000 小时内表现出稳定的锂沉积/剥离性能，而 LiFePO ₄ |HEMI-ASPE-Li|Li 全电池在 300 小时后表现出高容量保持率（≈96%）周期。这项工作贡献了一种创新的设计理念，为 ASPE 引入了高熵超分子动态网络。

更新日期：2022-11-07

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