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

Title
Tetrathiafulvalene-based covalent organic frameworks as high-voltage organic cathodes for lithium batteries
Type
Article in International Scientific Journal
Year
2024
Authors
Gonçalo Valente
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Raquel Dantas
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Pedro Ferreira
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Rebecca Grieco
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Nagaraj Patil
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Ana Guillem-Navajas
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David Rodríguez-San Miguel
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Felix Zamora
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Roman Guntermann
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Thomas Bein
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Joao Rocha
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Helena Braga
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Karol Strutynski
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Manuel Melle-Franco
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Rebeca Marcilla
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Manuel Souto
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Journal
Vol. 12
ISSN: 2050-7488
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Authenticus ID: P-016-W6M
Abstract (EN): 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 (similar to 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. We report a series of 2D tetrathiafulvalene (TTF)-based COFs incorporating different organic linkers between the electroactive moieties that were investigated as p-type organic cathode materials for lithium-organic batteries.
Language: English
Type (Professor's evaluation): Scientific
No. of pages: 9
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