A Pyrene-4,5,9,10-Tetraone-Based Covalent Organic Framework Delivers High Specific Capacity as a Li-Ion Positive Electrode



Gao, Hui, Neale, Alex R ORCID: 0000-0001-7675-5432, Zhu, Qiang, Bahri, Mounib ORCID: 0000-0002-8336-9158, Wang, Xue, Yang, Haofan, Xu, Yongjie, Clowes, Rob, Browning, Nigel D ORCID: 0000-0003-0491-251X, Little, Marc A
et al (show 2 more authors) (2022) A Pyrene-4,5,9,10-Tetraone-Based Covalent Organic Framework Delivers High Specific Capacity as a Li-Ion Positive Electrode. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 144 (21). pp. 9434-9442.

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Abstract

Electrochemically active covalent organic frameworks (COFs) are promising electrode materials for Li-ion batteries. However, improving the specific capacities of COF-based electrodes requires materials with increased conductivity and a higher concentration of redox-active groups. Here, we designed a series of pyrene-4,5,9,10-tetraone COF (PT-COF) and carbon nanotube (CNT) composites (denoted as PT-COFX, where <i>X</i> = 10, 30, and 50 wt % of CNT) to address these challenges. Among the composites, PT-COF50 achieved a capacity of up to 280 mAh g<sup>-1</sup> as normalized to the active COF material at a current density of 200 mA g<sup>-1</sup>, which is the highest capacity reported for a COF-based composite cathode electrode to date. Furthermore, PT-COF50 exhibited excellent rate performance, delivering a capacity of 229 mAh g<sup>-1</sup> at 5000 mA g<sup>-1</sup> (18.5C). Using <i>operando</i> Raman microscopy the reversible transformation of the redox-active carbonyl groups of PT-COF was determined, which rationalizes an overall 4 e<sup>-</sup>/4 Li<sup>+</sup> redox process per pyrene-4,5,9,10-tetraone unit, accounting for its superior performance as a Li-ion battery electrode.

Item Type: Article
Divisions: Faculty of Science and Engineering > School of Engineering
Faculty of Science and Engineering > School of Physical Sciences
Depositing User: Symplectic Admin
Date Deposited: 07 Jul 2022 11:39
Last Modified: 18 Jan 2023 20:56
DOI: 10.1021/jacs.2c02196
Open Access URL: https://doi.org/10.1021/jacs.2c02196
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URI: https://livrepository.liverpool.ac.uk/id/eprint/3157941