Intermolecular Chemistry in High-Entropy Solid Polymer Electrolyte Enabling Room Temperature Solid-State Lithium Metal Batteries
Hui-Juan Guo, Rui Shu, Yaxin Xie, Xueying Wang, Haonan Wu, Yuexian Song, Jianxin Tian, Fanpeng Cheng, Yangyang Guo*, Tingyu Zhu, Lijuan Shi*, Rui Wen, Qun Yi*
10.1039/d5ta03675e
Abstract: Solid polymer electrolytes with excellent processivity have attracted tremendous attention in advanced solid-state lithium metal batteries (SSLMBs), while their application remains a tough challenge due to the trade-off between high ionic conductivity and well mechanical strength. Here, via in situ polymerization, the unique Li+ solvation structures as well as abundant hydrogen bonds are inserted into a high-entropy supramolecular zwitterion solid polymer electrolyte (HESZ-SPE), significantly facilitating Li+ transport and improving mechanical properties at room temperature (RT). The in situ polymerized HESZ-SPE exhibits high electrochemical stability and excellent interfacial stability, and thus implements the uniform Li+ plating/stripping that revealed by COMSOL simulation. Remarkably, the HESZ-SPE achieves the balance in excellent mechanical strength, high ionic conductivity (4.60 × 10-3 S cm−1), an appreciable Li+ transference number (0.86) for RT SSLMBs. Consequently, the HESZ-SPE provides an excellent cycling stability, high coulombic efficiency and favorable rate capability at RT in SSLMBs, holding great promise in enabling high-performance electrochemical energy storage
具有优异加工性能的固态聚合物电解质在先进的固态锂金属电池（SSLMBs）中引起了广泛关注，然而其应用仍面临挑战，主要在于高离子电导率与良好机械强度之间存在相互制约的关系。本文通过原位聚合的方法，将独特的Li⁺溶剂化结构和丰富的氢键引入一种高熵超分子两性离子固态聚合物电解质（HESZ-SPE）中，显著促进了Li⁺的传输并改善了其在室温下的力学性能。原位聚合的HESZ-SPE表现出高的电化学稳定性与优异的界面稳定性，COMSOL模拟进一步证实其能够实现均匀的Li⁺沉积/剥离行为。值得注意的是，HESZ-SPE在室温下实现了优异的机械强度、高离子电导率（4.60 × 10⁻³ S cm⁻¹）以及可观的Li⁺迁移数（0.86），为室温固态锂金属电池提供了良好的循环稳定性、高库伦效率和优异的倍率性能。因此，HESZ-SPE在实现高性能电化学储能器件方面展现出巨大潜力。
