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Synthesis of Ionic Liquid Based Electrolytes, Assembly of Li-ion Batteries, and Measurements of Performance at High Temperature

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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.

Keywords:

Li‐organic batteries TEMPO radical organic batteries organic cathodes redox‐active covalent organic frameworks

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Solid-state Graft Copolymer Electrolytes for Lithium Battery Applications

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Published on: August 12, 2013

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.