Revealing the Mg-Ion Storage Mechanism within a Covalent Organic Framework Electrode



Wright, MA ORCID: 0000-0003-0617-3992, Neale, AR ORCID: 0000-0001-7675-5432, Acín-Lalanza, A, Gao, H, Rosseinsky, MJ ORCID: 0000-0002-1910-2483, Cooper, AI ORCID: 0000-0003-0201-1021 and Hardwick, LJ ORCID: 0000-0001-8796-685X
(2025) Revealing the Mg-Ion Storage Mechanism within a Covalent Organic Framework Electrode ACS Applied Energy Materials, 8 (22). pp. 16451-16456. ISSN 2574-0962, 2574-0962

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Abstract

Magnesium batteries offer a promising alternative to lithium-ion systems, but suitable electrodes remain limited. Covalent organic frameworks (COFs) are attractive candidates due to their structural tunability and open channels for ion transport. We report a pyrene- 4,5,9,10-tetraone COF composite with carbon nanotubes as a Mg electrode, delivering 70 mAh g–1at 200 mA g–1and operating at 1.3 V. In situ Raman spectroscopy confirms carbonyl-centered redox on pyrene tetraone, supporting a Mg2+-driven carbonyl reduction. Compared with Li+, only partial carbonyl utilization occurs, attributed to steric and electrostatic constraints of divalent Mg2+. This incomplete conversion to magnesium-enolate inspires future work toward structural optimization.

Item Type: Article
Uncontrolled Keywords: Covalent Organic Framework, <italic>In Situ</italic> Raman, Mg Battery, Battery Materials, Organic Electrodes, Raman Spectroscopy
Divisions: Faculty of Science & Engineering
Faculty of Science & Engineering > School of Physical Sciences
Faculty of Science & Engineering > School of Physical Sciences > Chemistry
Depositing User: Symplectic Admin
Date Deposited: 02 Dec 2025 16:20
Last Modified: 28 Feb 2026 14:33
DOI: 10.1021/acsaem.5c03247
Open Access URL: https://doi.org//10.1021/acsaem.5c03247
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URI: https://livrepository.liverpool.ac.uk/id/eprint/3195789
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