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

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

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

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.

As the demand for high-energy-density and safer energy storage technologies continues to grow, solid-state lithium metal batteries (SSLMBs) have emerged as one of the most promising candidates for next-generation batteries. However, the practical deployment of SSLMBs is still hindered by challenges such as poor mechanical strength of electrolytes, unstable electrode–electrolyte interfaces, and lithium dendrite growth. Recently, researchers from Northwestern Polytechnical University and Beijing Forestry University, led by Professor Ying Huang and Professor Zheng Zhang, reported a novel asymmetric composite solid-state electrolyte design that enables stable and high-performance solid-state lithium metal batteries. 

Why Advanced Solid-State Electrolytes Matter

  • Enhanced Safety: Solid-state electrolytes replace flammable liquid electrolytes, greatly improving battery safety while enabling the use of lithium metal anodes with extremely high theoretical capacity. 
  • Higher Energy Density: Lithium metal anodes offer a theoretical specific capacity of 3860 mAh g-1, which can significantly increase the energy density of next-generation batteries. 
  • Interface Stability: A well-designed solid electrolyte can simultaneously stabilize both the lithium metal anode interface and the high-voltage cathode interface, enabling long-term cycling stability. 

Innovative Design and Structural Features

  • Cellulose@MOF Scaffold: The researchers constructed a three-dimensional cellulose framework decorated with self-assembled metal–organic framework (MOF) nanosheets, forming a CP@MOF network that enhances both mechanical strength and ion transport. 
  • High Mechanical Strength: The electrolyte achieves a Young’s modulus of about 1.19 GPa, providing a strong mechanical barrier that effectively suppresses lithium dendrite penetration. 
  • Efficient Ion Transport: The MOF nanosheets anchor TFSI- anions and create fast Li+ transport pathways within the cellulose network, improving ionic conductivity and Li+ transference number. 
  • Asymmetric Electrolyte Architecture: An asymmetric composite solid-state electrolyte (ACSE) design is adopted to independently optimize the interfaces for both the lithium metal anode and high-voltage cathode. 

Applications and Future Outlook

  • Long-Term Cycling Stability: Lithium symmetric cells equipped with the designed electrolyte exhibit stable lithium plating and stripping for more than 5000 hours, indicating excellent dendrite suppression capability. 
  • High-Performance Full Cells: NCM811|Li full cells demonstrate stable cycling with 84.9% capacity retention after 350 cycles, confirming the effectiveness of the asymmetric electrolyte design. 
  • Practical Pouch Cell Demonstration: The assembled pouch cell delivers a high energy density of 337.9 Wh kg-1 and 711.7 Wh L-1, showing strong potential for real-world applications. 
  • Robust Mechanical Stability: Even under bending, cutting, or piercing conditions, the pouch cell remains operational, demonstrating excellent structural robustness and safety. 

This work demonstrates a mechano-electrochemical synergistic strategy for designing advanced solid-state electrolytes. By integrating a cellulose-MOF scaffold with asymmetric electrolyte architecture, the study provides a promising pathway toward high-energy-density and safe solid-state lithium metal batteries, bringing next-generation energy storage technologies closer to practical implementation.

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Electrochemistry
Physical Sciences > Chemistry > Physical Chemistry > Electrochemistry
Batteries
Physical Sciences > Materials Science > Materials for Energy and Catalysis > Batteries
Nanoscale Design, Synthesis and Processing
Physical Sciences > Materials Science > Nanotechnology > Nanoscale Design, Synthesis and Processing
Metal-organic Frameworks
Physical Sciences > Chemistry > Materials Chemistry > Metal-organic Frameworks
Materials for Energy and Catalysis
Physical Sciences > Materials Science > Materials for Energy and Catalysis
  • Nano-Micro Letters Nano-Micro Letters

    Nano-Micro Letters is a peer-reviewed, international, interdisciplinary and open-access journal that focus on science, experiments, engineering, technologies and applications of nano- or microscale structure and system in physics, chemistry, biology, material science, and pharmacy.