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

IF 11.2 1区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY

Journal of Materials Science & Technology Pub Date : 2025-06-22 DOI:10.1016/j.jmst.2025.04.075

Zhiyuan Lin, Yunhang Li, Wenbin Zhang, Guanghua Guo, Weihan Chen, Li Zhang, Shanran Yang, Yonggao Xia, Guofa Cai

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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.

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具有增强界面兼容性的终端功能化聚合物电解质，用于坚固的固态锂金属电池

具有高压阴极的固态锂金属电池（sslmb）为下一代储能技术提供了巨大的潜力，但面临着氧化稳定性差和聚合物电解质（PEs）界面不相容的挑战。本文设计了具有链聚合物骨架的末端功能化聚合物电解质（TFPEs），以增强其抗氧化性和界面相容性。在聚合物链末端引入吸电子基团异氰酸酯（-NCO），消除了末端羟基（-OH），增强了PEs的界面相容性和抗氧化分解能力。末端功能化聚（1,6-己二醇）碳酸二醇聚合物电解质（TFPCDL）具有良好的电化学稳定性，宽电化学稳定窗口（4.7 V）和高离子电导率（3.75 × 10−4 S cm−1,25°C）。采用TFPCDL的电池在充电至4.5 V时，循环100次后的容量保持率为88%，表现出稳定的循环性能。这项工作不仅为设计抗氧化聚乙烯提供了一种有前途的策略，而且加速了先进阴极材料sslmb的实际应用。

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来源期刊

Journal of Materials Science & Technology 工程技术-材料科学：综合

CiteScore

20.00

自引率

11.00%

发文量

995

审稿时长

13 days

期刊介绍： Journal of Materials Science & Technology strives to promote global collaboration in the field of materials science and technology. It primarily publishes original research papers, invited review articles, letters, research notes, and summaries of scientific achievements. The journal covers a wide range of materials science and technology topics, including metallic materials, inorganic nonmetallic materials, and composite materials.