Issue 36, 2024

Tetrathiafulvalene-based covalent organic frameworks as high-voltage organic cathodes for lithium batteries

Abstract

Redox-active covalent organic frameworks (COFs) are promising electrode materials for metal-ion batteries owing to their tunable electrochemical properties, adjustable structure, and resource availability. Herein, we report a series of two-dimensional tetrathiafulvalene (TTF)-based COFs incorporating different organic linkers between the electroactive moieties. These COFs were investigated as p-type organic cathode materials for lithium-organic batteries. The electrical conductivity of both neutral and doped TTF-COFs was measured using a van der Pauw setup, and their electronic structures were investigated through quantum-chemical calculations. Binder-free buckypaper TTF-based electrodes were prepared and systematically tested as organic cathodes in lithium half-cells. The results revealed high average discharge potentials (∼3.6 V vs. Li/Li+) and consistent cycling stability (80% capacity retention after 400 cycles at 2C) for the three TTF-COF electrodes. In addition, the specific capacity, rate capability, and kinetics varied depending on the structure of the framework. Our results highlight the potential of TTF-COFs as high-voltage organic cathodes for metal-ion batteries and emphasize the importance of molecular design in optimizing their electrochemical performance.

Graphical abstract: Tetrathiafulvalene-based covalent organic frameworks as high-voltage organic cathodes for lithium batteries

Supplementary files

Article information

Article type
Paper
Submitted
02 jul 2024
Accepted
09 aug 2024
First published
09 aug 2024
This article is Open Access
Creative Commons BY license

J. Mater. Chem. A, 2024,12, 24156-24164

Tetrathiafulvalene-based covalent organic frameworks as high-voltage organic cathodes for lithium batteries

G. Valente, R. Dantas, P. Ferreira, R. Grieco, N. Patil, A. Guillem-Navajas, D. Rodríguez-San Miguel, F. Zamora, R. Guntermann, T. Bein, J. Rocha, M. H. Braga, K. Strutyński, M. Melle-Franco, R. Marcilla and M. Souto, J. Mater. Chem. A, 2024, 12, 24156 DOI: 10.1039/D4TA04576A

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