Terminally functionalized polymer electrolytes with enhanced interfacial compatibility for robust solid-state lithium metal batteries

doi:10.1016/j.jmst.2025.04.075

J. Mater. Sci. Technol. ›› 2026, Vol. 247: 119-129.DOI: 10.1016/j.jmst.2025.04.075

• Research article • Previous Articles Next Articles

Terminally functionalized polymer electrolytes with enhanced interfacial compatibility for robust solid-state lithium metal batteries

Zhiyuan Lin^a,b,*, Yunhang Li^b, Wenbin Zhang^c, Guanghua Guo^d, Weihan Chen^b, Li Zhang^e, Shanran Yang^b, Yonggao Xia^b,d,*, Guofa Cai^a,*

^aKey Laboratory for Special Functional Materials of Ministry of Education, National & Local Joint Engineering Research Center for High-Efficiency Display and Lighting Technology, School of Nanoscience and Materials Engineering, Henan University, Kaifeng 475004, China;
^bSchool of New Energy, Ningbo University of Technology, Ningbo 315336, China;
^cInstitute of Engineering Thermophysics, School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China;
^dNingbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo 315201, China;
^eDepartment of Chemistry, Lishui University, Lishui 323000, China

Received:2025-01-17 Revised:2025-04-12 Accepted:2025-04-22 Published:2026-03-10 Online:2026-03-23
Contact: ^*E-mail addresses: lzhy@nbut.edu.cn (Z. Lin), xiayg@nimte.ac.cn (Y. Xia), caiguofa@henu.edu.cn (G. Cai).

Abstract

Abstract: Solid-state lithium metal batteries (SSLMBs) with high-voltage cathodes offer significant potential for next-generation energy storage but face challenges related to poor oxidative stability and interfacial incompatibility of polymer electrolytes (PEs). Herein, terminally functionalized polymer electrolytes (TFPEs) with chain polymer backbones were designed to enhance the antioxidation resistance and interfacial compatibility. Introduced the electron-withdrawing group of isocyanate (-NCO) at the end of the polymer chain to eliminate the end hydroxy (-OH), which can enhance the interfacial compatibility and antioxidative decomposition capacity for PEs. The terminally functionalized poly (1,6-hexanediol) carbonate diols polymer electrolytes (TFPCDL) deliver good electrochemical stability, wide electrochemical stability window (4.7 V), and high ionic conductivity (3.75 × 10^-4 S cm^-1 at 25 °C). Batteries employing TFPCDL demonstrated stable cycling performance with 88 % capacity retention after 100 cycles when charged to 4.5 V. This work not only highlights a promising strategy for designing antioxidative PEs but also accelerates the practical application of SSLMBs with advanced cathode materials.

Key words: Polymer electrolytes, Segment structure, Molecular design, Terminally functionalization, Interface compatibility

Zhiyuan Lin, Yunhang Li, Wenbin Zhang, Guanghua Guo, Weihan Chen, Li Zhang, Shanran Yang, Yonggao Xia, Guofa Cai. Terminally functionalized polymer electrolytes with enhanced interfacial compatibility for robust solid-state lithium metal batteries[J]. J. Mater. Sci. Technol., 2026, 247: 119-129.

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Terminally functionalized polymer electrolytes with enhanced interfacial compatibility for robust solid-state lithium metal batteries

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