Enhancing Lithium-Ion Flux Redistribution in Dendrite-Free Lithium-Sulfur Batteries Using Engineered Covalent Organic Frameworks

Enhancing

Engineering Covalent Organic Frameworks to Enhance Interfacial Lithium-Ion Flux Redistribution in Dendrite-Free Lithium-Sulfur Batteries

Tianli Li, Hua Hao, Jian Wang, Zhongzhi Yuan, Zhiyong Yu, and Hanxing Liu
Journal of Materials Chemistry A

Abstract

The quest for high-performance electrocatalysts that can efficiently adsorb and rapidly convert polysulfides is crucial for improving the specific capacity and cycling life of lithium-sulfur (Li-S) batteries. However, the performance of these batteries is often limited by the shuttling effect of lithium polysulfides (LiPSs) and the slow kinetics of redox reactions.

In this study, we introduce covalent organic frameworks (designated as fBTTP-COF), synthesized through a Schiff-base condensation reaction at room temperature. This method avoids the risks associated with solvothermal techniques. The fBTTP-COF serves as a porous π-conjugated structural material, featuring an ion-sieving architecture that facilitates rapid charge transfer and lithium-ion migration. Additionally, it possesses numerous anchoring sites along its π-conjugated backbone, which can effectively adsorb and promote the conversion of polysulfides.

Thanks to its remarkable catalytic properties, batteries equipped with fBTTP-COF modified separators demonstrate excellent cycle stability, showing a minimal capacity decay rate of just 0.037% over 700 cycles at 1C. These batteries also achieve a notable areal capacity of 5.59 mA h cm−2 with a high sulfur loading of 5 mg cm−2. Furthermore, Li//Li symmetric batteries exhibit stable lithium plating and stripping cycling over 483 hours.

This research provides a fresh perspective on the design of cost-effective catalysts aimed at enhancing the cycling life of Li-S batteries.

Article Information

DOI: 10.1039/D4TA08847F
Article Type: Paper
Submitted: December 12, 2024
Accepted: February 10, 2025
First Published: February 14, 2025

Citation

Li, T., Hao, H., Wang, J., Yuan, Z., Yu, Z., & Liu, H. (2025). Engineering covalent organic frameworks to enhance interfacial lithium-ion flux redistribution in dendrite-free lithium–sulfur batteries. Journal of Materials Chemistry A, Advance Article. DOI: 10.1039/D4TA08847F

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