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Vol. 18 (2026)

Mechano-Electrochemical Synergy in Cellulose@MOF Scaffold-Based Asymmetric Electrolyte for Stable Solid-State Lithium Metal Batteries

https://doi.org/10.1007/s40820-025-02039-x
Wanqing Fan
The MOE Key Laboratory of Material Physics and Chemistry Under Extraordinary Conditions, Ministry of Education, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xian 710072, People’s Republic of China
Xuetao Shi
The MOE Key Laboratory of Material Physics and Chemistry Under Extraordinary Conditions, Ministry of Education, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xian 710072, People’s Republic of China
Ying Huang
The MOE Key Laboratory of Material Physics and Chemistry Under Extraordinary Conditions, Ministry of Education, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xian 710072, People’s Republic of China
Kaihang She
The MOE Key Laboratory of Material Physics and Chemistry Under Extraordinary Conditions, Ministry of Education, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xian 710072, People’s Republic of China
Bowei Song
The MOE Key Laboratory of Material Physics and Chemistry Under Extraordinary Conditions, Ministry of Education, School of Chemistry and Chemical Engineering, Northwestern Polytechnical University, Xian 710072, People’s Republic of China
Zheng Zhang
State Key Laboratory of Efficient Production of Forest Resources, Beijing Key Laboratory of Lignocellulosic Chemistry, Beijing Forestry University, Beijing 100083, People’s Republic of China

Corresponding Author: Zheng Zhang

zhengzhang0527@163.com

Nano-Micro Letters, Vol. 18 (2026), Article Number: 208

Abstract

The application of polymer electrolytes is expected to revitalize solid-state lithium metal batteries (SSLMBs) with high energy density and enhanced safety. However, practical deployment faces challenges from inadequate mechanical properties of electrolyte and unstable interfaces in high-voltage SSLMBs. Herein, we design an asymmetric composite solid-state electrolyte (ACSE) composed of a cellulose framework in situ self-assembled with zeolitic imidazolate framework nanosheets (CP@MOF) embedded in a polymer matrix. The CP@MOF network provides the electrolyte with an elastic modulus of 1.19 GPa, effectively resisting Li dendrite penetration. Furthermore, theoretical calculations guided the compositional design of ACSE to address asynchronous interfacial requirements at cathode/electrolyte and anode/electrolyte interfaces, facilitating stable interphase formation and thus ensuring prolonged cycling of SSLMBs. Consequently, Li symmetric cells achieve extended cycling stability (> 5000 h) with minimal polarization. The NCM811|Li full cell maintains 84.9% capacity retention after 350 cycles. Notably, assembled NCM811 pouch cells deliver practical energy densities of 337.9 Wh kg−1 and 711.7 Wh L−1, demonstrating exceptional application potential. This work provides novel insights into the application of ACSEs for high-energy–density SSLMBs.


Highlights:
1 A structurally simple asymmetric solid-state electrolyte successfully stabilizes the interface between lithium metal and high-voltage cathodes in solid-state lithium metal batteries.
2 Environmentally friendly cellulose provides high mechanical support, while layered self-assembled metal–organic frameworks restrict TFSI⁻, efficiently promoting Li⁺ transport.
3 The assembled pouch cell exhibited a high gravimetric/volume energy density of 337.9 Wh kg−1/711.7 Wh L−1.

Keywords

Solid-state lithium metal batteries Asymmetric composite solid-state electrolyte Elastic modulus Pouch cells
Fan, Wanqing, Xuetao Shi, Ying Huang, Kaihang She, Bowei Song, and Zheng Zhang. 2026. “Mechano-Electrochemical Synergy in Cellulose@MOF Scaffold-Based Asymmetric Electrolyte for Stable Solid-State Lithium Metal Batteries”. Nano-Micro Letters 18 (January):208. https://doi.org/10.1007/s40820-025-02039-x.
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