Citation: Kehan Tang, Peiwen Xu, Xinyuan Wu, Youlong Zhu. In situ growth of redox-active covalent organic frameworks on aminated MXene for functional separator coatings in lithium-sulfur batteries[J]. Chinese Chemical Letters, ;2026, 37(8): 111883. doi: 10.1016/j.cclet.2025.111883 shu

In situ growth of redox-active covalent organic frameworks on aminated MXene for functional separator coatings in lithium-sulfur batteries

Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education, IGCME, School of Chemistry, Sun Yat-sen University, Guangzhou 510006, China

zhuyl9@mail.sysu.edu.cn

Received Date: 25 July 2025
Revised Date: 16 September 2025
Accepted Date: 23 September 2025
Available Online: 23 September 2025

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Lithium-sulfur (Li-S) batteries are considered as one of the most promising next-generation energy storage systems owing to their high theoretical capacity and energy density. However, conventional polyolefin-based separators suffer from randomly distributed pores with broad size distributions, which are ineffective in suppressing the polysulfide shuttle effect. Moreover, they lack functional groups for catalyzing polysulfides conversion and promoting uniform lithium-ion deposition. Herein, we synthesized a hybrid material (denoted as DAAQ-TFP/MXene) via in situ growth of redox-active covalent organic frameworks (DAAQ-TFP) on amine-functionalized MXene nanosheets. The resulting DAAQ-TFP/MXene hybrid features a porous architecture and dual binding/catalytic sites, enabling efficient polysulfides adsorption and catalytic conversion, enhanced lithium-ion transport, and uniform lithium deposition. Consequently, the DAAQ-TFP/MXene-coated PP separator exhibits a high lithium-ion transference number (0.53). The LiLi symmetric cell incorporating this separator operates stably for 3800 h at 5 mA/cm² and 1 mAh/cm². Furthermore, Li-S full cells using DAAQ-TFP/MXene@PP separator delivers a high specific capacity (1224 mAh/g at 0.1 C), excellent rate performance (631 mAh/g at 5 C), and long-term cycling stability (71.3% capacity retention after 300 cycles at 1 C). This study provides a promising strategy for designing MXene-COF hybrid materials as functional coatings to improve the performance of Li-S batteries.
- Covalent organic frameworks,
- Functional coating,
- Separator,
- Lithium-sulfur batteries,
- Hybrid materials,
- MXene
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