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Vol. 18 (2026)

Regulating Li+ Transport and Interfacial Stability with Zwitterionic COF Protective Layer Towards High-Performance Lithium Metal Batteries

https://doi.org/10.1007/s40820-025-02017-3
Liya Rong
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China
Yifeng Han
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China
Chi Zhang
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China
Hongling Yao
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China
Zhaojun He
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China
Xianbao Wang
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China
Zaiping Guo
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China
Tao Mei
Hubei Collaborative Innovation Center for Advanced Organic Chemical Materials, Overseas Expertise Introduction Center for Discipline Innovation (D18025), Key Laboratory for the Green Preparation and Application of Functional Materials, Hubei Key Laboratory of Polymer Materials, College of New Energy and Electrical Engineering, Hubei University, Wuhan 430062, People’s Republic of China

Corresponding Author: Tao Mei

meitao@hubu.edu.cn

Nano-Micro Letters, Vol. 18 (2026), Article Number: 163

Abstract

The sluggish Li+ migration kinetics and unstable electrode/electrolyte interface severely hinder the commercial application of high-performance lithium metal batteries (LMBs). Herein, an artificial protective layer is constructed using zwitterionic covalent organic framework (Z-COF) simultaneously containing sulfonate and ethidium groups, aiming to facilitate rapid, uniform Li+ transport and stabilize anode interface. The sulfonate groups with high lithiophilicity provide abundant hopping sites for fast Li+ diffusion. The ethidium cations immobilize TFSI− and solvent molecules by ion–dipole interactions, which accelerate the dissociation of LiTFSI and Li+ desolvation. Moreover, the monodispersed zwitterionic units coupling with ordered micropore structures in Z-COF create exclusive Li+ migration channels, modulate homogeneous space charge distribution, kinetically facilitating uniform Li+ deposition. Experiments and theoretical calculations indicate that C–F and S–N bonds of TFSI− exhibit enhanced cleavage susceptibility driven by electrostatic attraction, realizing a LiF/Li3N-rich electrolyte/electrode interface. The designed Z-COF protection layer enables Li|Li symmetrical cells stable cycling over 6300 h at 2 mA cm−2/2 mAh cm−2. The Z-COF@Li|LiFePO4 (LFP) full cells deliver high-capacity retention of 85.2% after 1000 cycles at 8 C. The assembled Z-COF@Li|LFP pouch cells demonstrate a lifespan of more than 240 cycles. This work provides fresh insights into the practical application of zwitterionic COF in next-generation LMBs.


Highlights:
1 Ethidium cations acted as “anion capturers” to immobilize TFSI−, which rendered the C-F and S-N bonds prone to cleavage, facilitating the formation of LiF/Li3N-rich solid electrolyte interphase.
2 Ion–dipole interaction between ethidium groups and dimethoxyethane/dioxolane, boosting Li+ desolvation.
3 Sulfonate groups exhibited an ion-sieving effect that selectively attracted Li⁺ while excluding TFSI⁻, promoting LiTFSI dissociation and accelerating Li+ migration.

Keywords

Zwitterionic covalent organic framework Li migration kinetic regulation Li desolvation Charge distribution Interface stability
Rong, Liya, Yifeng Han, Chi Zhang, Hongling Yao, Zhaojun He, Xianbao Wang, Zaiping Guo, and Tao Mei. 2026. “Regulating Li+ Transport and Interfacial Stability With Zwitterionic COF Protective Layer Towards High-Performance Lithium Metal Batteries”. Nano-Micro Letters 18 (January):163. https://doi.org/10.1007/s40820-025-02017-3.
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