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单离子传导共价有机框架在基于聚环氧乙烷的电解质中作为锂离子泵用于高性能固态锂硫电池。

Single-ion-conducted covalent organic framework serving as Li-ion pump in polyethylene oxide-based electrolyte for robust solid-state Li-S batteries.

作者信息

Zhang Jiaxue, Hu Ben, Zhu Acheng, Qi Yiming, Wang Yuyang, Han Shichang, Zhu Tianyu, Xu Jie

机构信息

College of Mechanical Engineering, Wanjiang University of Technology, Ma'anshan 243031, China.

College of Mechanical Engineering, Wanjiang University of Technology, Ma'anshan 243031, China.

出版信息

J Colloid Interface Sci. 2025 Jan 15;678(Pt B):105-113. doi: 10.1016/j.jcis.2024.08.255. Epub 2024 Sep 2.

DOI:10.1016/j.jcis.2024.08.255
PMID:39241441
Abstract

Poly(ethylene oxide) (PEO)-based electrolytes are widely used for building solid-state lithium-sulfur (Li-S) batteries but suffer from poor lithium-ion (Li) transportation kinetics. Here, a lithium-sulfonated covalent organic framework (TpPa-SOLi) was synthesized and functionalized as a Li pump in a PEO-based solid-state electrolyte to fabricate robust Li-S batteries. The designed TpPa-SO Li with its porous skeleton and abundant lithium sulfonate groups not only provided iontransport channels but also enhanced the fast migration of Li. The PEO composite electrolyte containing 5 %-TpPa-SOLi exhibited a notable ionic conductivity of 6.28 × 10 S cm and an impressive Li transference number of 0.78 at 60 °C. As a result, Li-Li symmetric batteries with the optimized PEO/TpPa-SOLi composite electrolyte stably cycled for 300 h, with a minimal overpotential of only 100 mV at 0.5 mA cm. Moreover, the customized solid-state Li-S batteries based on PEO/TpPa-SOLi were stable for 600 cycles at 60 C with a high Coulombic efficiency of approximately 98 %. This study provides a promising strategy for introducing covalent-organic-framework (COF)-based Li pumps to build robust solid-state Li-S batteries.

摘要

聚环氧乙烷(PEO)基电解质被广泛用于构建固态锂硫(Li-S)电池,但存在锂离子(Li)传输动力学较差的问题。在此,合成了一种锂磺化共价有机框架(TpPa-SOLi)并将其功能化作为PEO基固态电解质中的锂泵,以制造坚固的Li-S电池。设计的TpPa-SO Li具有多孔骨架和丰富的磺酸锂基团,不仅提供了离子传输通道,还增强了Li的快速迁移。含有5%-TpPa-SOLi的PEO复合电解质在60°C时表现出6.28×10 S cm的显著离子电导率和0.78的令人印象深刻的Li迁移数。结果,采用优化的PEO/TpPa-SOLi复合电解质的Li-Li对称电池稳定循环300小时,在0.5 mA cm时的最小过电位仅为100 mV。此外,基于PEO/TpPa-SOLi定制的固态Li-S电池在60°C下稳定循环600次,库仑效率约为98%。本研究为引入基于共价有机框架(COF)的锂泵来构建坚固的固态Li-S电池提供了一种有前景的策略。

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