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Redox-active covalent organic framework electrolyte modulates interfacial Li+ deposition for stable solid-state lithium metal batteries.

Created on 20 Jun 2026

Authors

Lina Zhang, Ruixiang Duan, Xu Liu, Qikai Wang, Lili Zhang

Published in

Journal of colloid and interface science. Volume 723. Pages 140961. Jun 16, 2026. Epub Jun 16, 2026.

Abstract

Solid polymer electrolytes (SPEs) have been widely recognized as promising candidates for safe and high-energy-density solid-state lithium metal batteries. Nevertheless, their practical application is hampered by critical challenges in mechanical properties, ionic transport and interfacial stability. In this work, a redox-active covalent organic framework (denoted as TNCOF) is proposed to modulate interfacial Li+ deposition behavior. The TNCOF featuring abundant carbonyls and triazine rings, not only facilitates Li salt dissociation and provides ordered ion conduction pathways but also regulates the local Li+ environment through its redox-active units. Consequently, the optimized composite polymer electrolyte (CPE-8%TNCOF) exhibits an excellent performance with an ionic conductivity of 8.35 × 10-4 S cm-1, a lithium-ion transfer number ( [Formula: see text] ) of 0.45. Moreover, the TNCOF promotes homogeneous Li nucleation and induces the formation of Li2O-rich solid electrolyte interphase (SEI). Impressively, the assembled all-solid-state LiS battery delivers a retention of 86.26% over 100 cycles at 0.2C. More notably, the LiFePO4|CPE-8%TNCOF|Li battery delivers a discharge capacity of 143 mA h g-1 after 400 cycles at 0.5C, corresponding to capacity retention of 93.46%, and maintains stable operation for 1000 cycles at 1C. This study provids new design ideas and reliable experimental basis for redox-mediated interfacial engineering in solid-state lithium metal batteries.

PMID:
42320131
Bibliographic data and abstract were imported from PubMed on 20 Jun 2026.

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