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In Situ Electrochemical Activation of Ti3C2Tx MXene as Positive Electrode Active Material for Rechargeable Aluminum Batteries
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DOI：10.1149/1945-7111/ae5c41.png)
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Abstract
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Two-dimensional metal carbides called MXenes have ability for reversible charge and discharge with the multivalent metal ions. However, the discharge capacity of Ti3C2Tx, the most common type of MXene, was very limited similar to 10 mAh g-1 as the positive electrode active material for rechargeable aluminum batteries (RABs). In this study, we investigated the in situ electrochemical activation process of Ti3C2Tx MXene in sulfone-based electrolytes with varying aluminum coordination states. Comprehensive electrochemical, spectroscopic, and structural analyses revealed that only the AlCl3-dimethyl sulfone (DMSO2) electrolyte enabled the progressive enhancement of redox activity through repeated potential cycling. NMR and Raman spectroscopy indicated the dominant formation of solvated Al(DMSO2)33+ species, while X-ray diffraction showed a distinct expansion of the MXene interlayer spacing from 1.23 nm to 1.52 nm after activation. These results demonstrate that the in situ activation originates from the reversible intercalation of strongly solvated Al3+ complexes, which dynamically widen the interlayer gap without significant structural degradation. Although the discharge capacity (similar to 100 mAh g-1) remains moderate, this study elucidates the key role of electrolyte-derived solvation structures in enabling redox activation of MXene materials, offering mechanistic insights for the rational design of aluminum battery electrodes.
Keywords:
batteries
interface modification
molten salts - low temperature molten salts
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3.3
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3.3W
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9.4W
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