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

TL;DR

A new cellulose and metal-organic framework-based electrolyte improves the stability and energy density of solid-state lithium metal batteries.

Contribution

The novel asymmetric electrolyte design combines cellulose and MOFs to stabilize lithium interfaces and achieve high energy density.

Findings

The electrolyte achieves 5000 hours of stable cycling in Li symmetric cells with minimal polarization.

NCM811|Li full cells retain 84.9% capacity after 350 cycles.

Pouch cells reach energy densities of 337.9 Wh/kg and 711.7 Wh/L.

Abstract

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

Environmentally friendly cellulose provides high mechanical support, while layered self-assembled metal–organic frameworks restrict TFSI⁻, efficiently promoting Li⁺ transport.

The assembled pouch cell exhibited a high gravimetric/volume energy density of 337.9 Wh kg−1/711.7 Wh L−1.

The online version contains supplementary material available at 10.1007/s40820-025-02039-x.

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.

The online version contains supplementary material available at 10.1007/s40820-025-02039-x.

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