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Updated: Jun 19, 2026
11:04
Synthesis of Ionic Liquid Based Electrolytes, Assembly of Li-ion Batteries, and Measurements of Performance at High Temperature
Published on: December 20, 2016
Electrolyte-Framework Matching in High-Voltage TEMPO-COF Cathodes for Lithium Batteries
Marilyn Esclance DMello1, Nagaraj Patil2, Fanni Fekecs1
1CiQUS, Centro Singular de Investigación en Química Biolóxica e Materiais Moleculares, Departamento De Química-Física, Universidade De Santiago de Compostela, Santiago de Compostela, Spain.
Advanced Science (Weinheim, Baden-Wurttemberg, Germany)
|June 18, 2026
Summary
High-voltage organic cathodes using TEMPO-based frameworks show promise for sustainable energy storage. Optimizing electrolyte anions, particularly LiDFOB, significantly enhances battery performance and achieves record mass loadings for TEMPO cathodes.
Area of Science:
- Materials Science
- Electrochemistry
- Sustainable Energy
Background:
- High-voltage organic cathodes are crucial for advanced energy storage solutions.
- TEMPO-based frameworks offer potential but face challenges in development and electrolyte interaction.
- Understanding electrolyte anion effects is key to improving performance.
Purpose of the Study:
- To develop and evaluate novel porous TEMPO-based covalent organic frameworks (COFs) for high-voltage organic cathodes.
- To investigate the impact of various electrolyte anions on the electrochemical performance of these COFs.
- To establish framework-electrolyte matching as a critical design principle for radical-functionalized organic battery materials.
Main Methods:
- Post-synthetic functionalization of imine-linked COFs with N3-TEMPO via click chemistry.
- Electrochemical evaluation of TEMPO-TB and TEMPO-TP COFs as cathodes in Li-organic batteries using different LiX electrolytes.
- Systematic analysis of anion-dependent electrochemical behavior, including capacity, rate capability, and cycling stability.
Main Results:
- Crystalline, porous TEMPO-TB and TEMPO-TP COFs with uniform redox sites were successfully synthesized.
- Both COFs demonstrated reversible p-type redox activity at high voltages (∼3.6-3.7 V vs. Li/Li+).
- LiDFOB electrolyte significantly outperformed others, showing enhanced capacity, rate capability, and stability due to favorable anion interactions.
- Binder-free electrodes achieved record mass loadings (40 mg cm-2) and areal capacity (1.3 mAh cm-2) for TEMPO cathodes.
Conclusions:
- Framework-electrolyte matching is a vital strategy for optimizing high-voltage TEMPO-based organic cathodes.
- LiDFOB electrolyte offers superior performance characteristics for these systems.
- The developed TEMPO-COFs and optimized electrolyte combinations represent a significant advancement in sustainable energy storage materials.
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