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

**Authors:** Matthew A. Wright, Alex R. Neale, Andrés Acín-Lalanza, Hui Gao, Matthew J. Rosseinsky, Andrew I. Cooper, Laurence J. Hardwick

PMC · DOI: 10.1021/acsaem.5c03247 · 2025-11-07

## TL;DR

This paper explores a new COF-based electrode for magnesium batteries, revealing how Mg ions are stored and how structural limitations affect performance.

## Contribution

The study introduces a COF composite electrode and provides insights into the Mg-ion storage mechanism through in situ Raman spectroscopy.

## Key findings

- The COF composite delivers 70 mAh g–1 at 200 mA g–1 with a 1.3 V operating voltage.
- In situ Raman confirms carbonyl-centered redox reactions driven by Mg2+.
- Steric and electrostatic constraints limit carbonyl utilization compared to Li+.

## 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–1 at 200 mA g–1 and 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.

## Linked entities

- **Chemicals:** Mg (PubChem CID 888), Li+ (PubChem CID 28486), Mg2+ (PubChem CID 888)

## Full-text entities

- **Chemicals:** Mg2+ (-), COFs (MESH:D000073396), carbon nanotubes (MESH:D037742), Magnesium (MESH:D008274), Li+ (MESH:D008094)

## Figures

5 figures with captions in the complete paper: https://tomesphere.com/paper/PMC12648465/full.md

---
Source: https://tomesphere.com/paper/PMC12648465