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Engineering 4-Connecting 3D Covalent Organic Frameworks with Oriented Li+ Channels for High-Performance Solid-State
Yanan Zhang1,2, Chi Shan1,2, Zhuo Chen1,2
1Key Laboratory of Chemical Additives for China National Light Industry, College of Chemistry and Chemical Engineering, Shaanxi University of Science and Technology, Xi'an, 710021, P. R. China.
Small (Weinheim an Der Bergstrasse, Germany)
|April 22, 2025
Summary
New covalent organic frameworks (COFs) enhance ion conductivity in solid-state electrolytes for stable lithium metal batteries. These materials improve lithium-ion transport and anode stability, enabling long-lasting battery performance.
Area of Science:
- Materials Science
- Electrochemistry
- Polymer Science
Background:
- Solid-state electrolytes (SSEs) are crucial for high-performance lithium metal batteries (LMBs).
- Covalent organic frameworks (COFs) offer potential as Li-ion conductors due to their structure and tunability.
- Existing COFs face limitations in active sites and segmental motion, hindering ionic conductivity.
Purpose of the Study:
- To design and synthesize novel 3D porous COF frameworks for enhanced Li+ transport in SSEs.
- To improve the stability and performance of lithium anodes in LMBs.
- To investigate the structure-property relationships governing Li+ conduction in COFs.
Main Methods:
- Synthesis of 3D porous COF frameworks (TP-COF and TB-COF) using linear ditopic monomers.
- Integration of COFs with polymer electrolytes to form SSEs.
- Electrochemical characterization of SSEs, including ionic conductivity and Li+ transference number measurements.
- Cell assembly and cycling tests using LiFePO4 (LFP) cathodes and Li metal anodes.
- Molecular dynamics simulations and COMSOL Multiphysics modeling.
Main Results:
- TB-COF exhibits superior Li+ conduction (8.89 × 10-4 S cm-1) and a high transference number (0.80) due to larger pores and abundant active sites.
- PEO-TB-COF SSEs demonstrate over 1000 hours of stability at 1 mA cm-2 and retain 90% capacity after 800 cycles in LFP||Li cells.
- A LiF/Li3N-rich solid electrolyte interphase (SEI) promotes uniform Li deposition.
- Simulations confirm extended Li+ transport channels and reduced interfacial barriers contribute to enhanced performance.
Conclusions:
- The developed 3D porous COFs, particularly TB-COF, significantly enhance Li+ transport and stabilize lithium anodes in LMBs.
- The rational design of COF architecture and active sites is key to overcoming limitations in ionic conductivity.
- These findings pave the way for advanced SSEs for next-generation high-performance and safe lithium metal batteries.
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