Intermolecular chemistry in high-entropy solid polymer electrolytes enabling room temperature solid-state lithium metal batteries

Abstract

Solid polymer electrolytes with excellent processability 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 good 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 promotes the uniform Li+ plating/stripping 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), and an appreciable Li+ transference number (0.86) for RT SSLMBs. Consequently, the HESZ-SPE provides excellent cycling stability, high coulombic efficiency and favorable rate capability at RT in SSLMBs, holding great promise in enabling high-performance electrochemical energy storage.

Graphical abstract: Intermolecular chemistry in high-entropy solid polymer electrolytes enabling room temperature solid-state lithium metal batteries

Supplementary files

Article information

Article type
Paper
Submitted
08 May 2025
Accepted
01 Jul 2025
First published
02 Jul 2025

J. Mater. Chem. A, 2025, Advance Article

Intermolecular chemistry in high-entropy solid polymer electrolytes enabling room temperature solid-state lithium metal batteries

H. Guo, R. Shu, Y. Xie, X. Wang, H. Wu, Y. Song, J. Tian, F. Cheng, Y. Guo, T. Zhu, L. Shi, R. Wen and Q. Yi, J. Mater. Chem. A, 2025, Advance Article , DOI: 10.1039/D5TA03675E

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