Lamellar COF solid-state electrolytes for robust ambient-temperature lithium-ion transfer enhanced by PEI-driven channel alignment

Lamellar COF solid-state electrolytes for robust ambient-temperature lithium-ion transfer enhanced by PEI-driven channel alignment

Ionic covalent organic framework (COF) lamellar membranes are the alternative materials as promising Li+ conductors for all-solid-state lithium batteries. However, COF lamellar membrane suffers from poor structural stability and inevitable cross-layer transfer resistance due to the weak interaction...

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Bibliographic Details
Main Authors: Yafang Zhang, Xinji Zhang, Jiajia Huang, Zhirong Yang, Shiyue Zhou, Chenye Wang, Wenjia Wu, Jingtao Wang
Format: Article
Language:English
Published: KeAi Communications Co., Ltd. 2025-05-01
Series:Green Energy & Environment
Subjects:
Lamellar composite electrolyte
COF nanosheets
Polymer-driven channel alignment
Ionic conductivity
All-solid-state lithium battery
Online Access:http://www.sciencedirect.com/science/article/pii/S2468025724002784
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Summary:Ionic covalent organic framework (COF) lamellar membranes are the alternative materials as promising Li+ conductors for all-solid-state lithium batteries. However, COF lamellar membrane suffers from poor structural stability and inevitable cross-layer transfer resistance due to the weak interaction at interface of adjacent nanosheets. Herein, a lamellar polymer-threaded ionic COF (PEI@TpPa-SO3Li) composite electrolyte with single Li+ conduction was prepared by assembling lithium sulfonated COF (TpPa-SO3Li) nanosheets and then threading them with polyethyleneimine (PEI) chains. It reveals that the threaded PEI chains induce the oriented permutation of pore channel of PEI@TpPa-SO3Li electrolyte through electrostatic interaction between –NH2/−NH− and –SO3Li groups. This enables the construction of continuous and aligned –SO3− … Li+ … −NH2/−NH− pairs along pore channels, which act as efficient Li+ conducting sites and afford high Li+ hopping conduction (1.4 × 10−4 S cm−1 at 30 °C) with a high Young's modulus of 408.7 MP and wide electrochemical stability window of 0∼4.7 V. The assembled LiFePO4||Li and LiNi0.8Mn0.1Co0.1O2||Li half-cells achieve high discharge capacities of 155.0 mAh g−1 and 167.2 mAh g−1 at 30 °C under 0.2 C, respectively, with high capacity retention of 98% after 300 cycles. This study provides an alternative route to highly ion-conductive lamellar porous electrolytes for high-performance energy devices.
ISSN:2468-0257

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