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Vol. 16 (2024)

Covalent Organic Framework with 3D Ordered Channel and Multi-Functional Groups Endows Zn Anode with Superior Stability

https://doi.org/10.1007/s40820-023-01278-0
Bin Li
School of Chemical Engineering, North China University of Science and Technology, Tangshan 063009, People’s Republic of China
Pengchao Ruan
School of Materials Science and Engineering, Central South University, Changsha 410083, People’s Republic of China
Xieyu Xu
State Key Laboratory for Mechanical Behavior of Materials, Xi’an Jiaotong University, Xi’an 710049, People’s Republic of China
Zhangxing He
School of Chemical Engineering, North China University of Science and Technology, Tangshan 063009, People’s Republic of China
Xinyan Zhu
School of Chemical Engineering, North China University of Science and Technology, Tangshan 063009, People’s Republic of China
Liang Pan
School of Chemical Engineering, North China University of Science and Technology, Tangshan 063009, People’s Republic of China
Ziyu Peng
School of Chemical Engineering, North China University of Science and Technology, Tangshan 063009, People’s Republic of China
Yangyang Liu
State Key Laboratory for Mechanical Behavior of Materials, Xi’an Jiaotong University, Xi’an 710049, People’s Republic of China
Peng Zhou
Hunan Provincial Key Defense Laboratory of High Temperature Wear‑Resisting Materials and Preparation Technology, Hunan University of Science and Technology, Xiangtan 411201, People’s Republic of China
Bingan Lu
School of Physics and Electronics, Hunan University, Changsha 410082, People’s Republic of China
Lei Dai
School of Chemical Engineering, North China University of Science and Technology, Tangshan 063009, People’s Republic of China
Jiang Zhou
School of Materials Science and Engineering, Central South University, Changsha 410083, People’s Republic of China

Corresponding Author: Jiang Zhou

zhou_jiang@csu.edu.cn

Nano-Micro Letters, Vol. 16 (2024), Article Number: 76

Abstract

Achieving a highly robust zinc (Zn) metal anode is extremely important for improving the performance of aqueous Zn-ion batteries (AZIBs) for advancing “carbon neutrality” society, which is hampered by the uncontrollable growth of Zn dendrite and severe side reactions including hydrogen evolution reaction, corrosion, and passivation, etc. Herein, an interlayer containing fluorinated zincophilic covalent organic framework with sulfonic acid groups (COF-S-F) is developed on Zn metal (Zn@COF-S-F) as the artificial solid electrolyte interface (SEI). Sulfonic acid group (− SO3H) in COF-S-F can effectively ameliorate the desolvation process of hydrated Zn ions, and the three-dimensional channel with fluoride group (-F) can provide interconnected channels for the favorable transport of Zn ions with ion-confinement effects, endowing Zn@COF-S-F with dendrite-free morphology and suppressed side reactions. Consequently, Zn@COF-S-F symmetric cell can stably cycle for 1,000 h with low average hysteresis voltage (50.5 mV) at the current density of 1.5 mA cm−2. Zn@COF-S-F|MnO2 cell delivers the discharge specific capacity of 206.8 mAh g−1 at the current density of 1.2 A g−1 after 800 cycles with high-capacity retention (87.9%). Enlightening, building artificial SEI on metallic Zn surface with targeted design has been proved as the effective strategy to foster the practical application of high-performance AZIBs.


Highlights:
1 A fluorinated zincophilic covalent organic framework (COF-S-F) with sulfonic acid group (-SO3H) is prepared on the surface of Zn anode, which promotes the desolvation of hydrated Zn ions and inhibits the side reactions.
2 The highly electronegative -F group in COF-S-F promotes fast and uniform transport of Zn ions along the interconnected channels, which contributes to the uniform electrodeposition process of Zn metal.
3 Zn@COF-S-F symmetric cell achieves a superior stability of 1,000 h and Zn@COF-S-F|MnO2 cell delivers high specific capacity of 206.8 mAh g−1 at current density of 1.2 A g−1.

Keywords

Aqueous Zn ion batteries Covalent organic framework Interfacial modification Zn ion flux regulation Desolvation effect
Li, Bin, Pengchao Ruan, Xieyu Xu, Zhangxing He, Xinyan Zhu, Liang Pan, Ziyu Peng, Yangyang Liu, Peng Zhou, Bingan Lu, Lei Dai, and Jiang Zhou. 2024. “Covalent Organic Framework With 3D Ordered Channel and Multi-Functional Groups Endows Zn Anode With Superior Stability”. Nano-Micro Letters 16 (January):76. https://doi.org/10.1007/s40820-023-01278-0.
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